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z8@sBDNNxM+2SJXkOl*!$cBi_FbgE2wQHY*etfaKs`m#|^y7i#dso*lBDW8_nmk%=KTQ(umH8S@5Y1Qr zP$*EXFL$re3^2ybyPUx>({o7iJ(JAxXcZ`igTrBShB76n`KE_ma;QJ)WWnrtp9~wI zPg2_5wAWs)_Y~!}=S*SPw9+IaR#b$iXL1=vZ{Rx~+LmenC%6(hyDyvU7BMw_*0?iZ zP4b#Pq3R8J`fD@z*=>6+3im5&tzMykFeQCi4|#$+oFcSRea5afnmqxU zp=3M0C3usquYN-#=2(1AnK_9KXRrr~%livzgPq4Q9@zl}TAAnMvrgt5yd7eTWan0nTlBk}=Gdv~jQ_cbFG?uN|N|YT|E@!a+?Vnt5=x^9wI3|hz?T$oN z?#0TJ*PwC@VUJveQ@C-~!@v~1Pr6`bZ_#Y7kYASVSX?k}4(McV5=ai7`C}{CAFMs2qf>|HQ;SuwUh+!(_il!UO^GX>0@RoW1GoiVkhj?*YDM? z_7$#1y8R)MZNC!3&}>|@%hj^)Ma>DDor_m)g&cLwHG;q=yWIN1d(?s{wx_4H)-&w!G7s0%zOOJ5+6@3^PBb04}95YA*C?CmMJo-NG z)qR%8j znqLe?{Z*u>h~ulKu)N!OqMJcd=*Kvc3N^Z^dBPc|IByqKbv{P&tDbu8evVOU6?!#J z|LW@e^3|2H)2IGJ=+)zggK_5JM;pK{k={Zt0cDz;A2dMZ`e)6JCgxpgHz0nOI^|qb zm-=0gsQV8J2(IMzlS*6n6+aMhZ>5xc9&@k@&1OYh?)&hLY%-||n}mJaS^=slt`Q!nUM=m> rightPredicate[ - restriction - ]( - repeat(inputRules)) + dg.build().execute( + addSubset(inputGraphs) + >> rightPredicate[ + restriction + ]( + repeat(inputRules)) + ) ) - ) - \end{verbatim} + \end{lstlisting} Der durch die Regelanwendung erzeugte Hypergraph kann als über verschiedene print Befehle in einer Latex generierten PDF Datei dargestellt werden. Dafür muss ein FlowPrinter, DGPrinter oder GraphPrinter Objekt erzeugt werden \cite{mod}. - \begin{verbatim} + \begin{lstlisting} flowPrinter = FlowPrinter() flowPrinter.printUnfiltered = False postSection("Loaded Graphs") for a in inputGraphs: - a.print() + a.print() postSection("Loaded Rules") for a in inputRules: - a.print() + a.print() postSection("Product Graphs") for a in dg.vertices: - a.graph.print() - \end{verbatim} + a.graph.print() + \end{lstlisting} M\o{}d wurde verwendet die Einwirkung natürlich auftretenden Reaktionen auf natürliche oder synthetische Moleküle zu untersuchen. \section{networkx} Networkx ist ein Pythonbasiertes Netzwerk und Graphen Analyse Tool \cite{networkx}. Eine Funktion ist dabei das identifizieren aller sehnen losen Zyklen. Während der laufzeit des Graptransformationstools wurden verschiedene Analysen dieser sehnen losen Zyklen als restriction verwendet. @@ -680,7 +714,7 @@ \end{verbatim} Für den Vergleich wurden die selben Berechnungen für TMS durchgeführt. Die Kohlenstoff Verschiebung von TMS lag dabei bei 179.73 ppm. Die Bestimmung chemisch Äquivalenter Kerne wurde von Hand durchgeführt. Für jedes mit dem Graptransformationstool erzeugte Molekül wurde ein $^{13}$C-NMR berechnet. \section{NMR-Vergleich} - Um die von ORCA berechneten NMR Spektren zu Vergleichen und ihre Ähnlichkeit zu Quantifizieren wurde die Binning Methode mit anschließender Crosscorrelation angewandt \cite{nmrbin}. Jeder Peak $j$ des Spektrums setzt sich aus seiner Intensität $I_{j}$ und seiner Verschiebung $\nu_{j}$ zusammen. Zuerst wird für ein gegebenes NMR Spektrum der Peak mit der größten chemischen Verschiebung $\nu_{max}$ und der kleinsten chemischen Verschiebung $\nu_{min}$ bestimmt und eine Bingröße $b$ festgelegt. Der größte Wert $\nu_{max}$ wird dabei aufgerundet und um eine Bingröße $b$ erhöht (Gleichung \ref{binupper}). Der kleinste Wert $\nu_{min}$ wird abgerundet und um eine Bingröße $b$ verringert (Gleichung \ref{binlower}). + Um die von dem quatntenchemischen berechneten NMR Spektren zu Vergleichen und ihre Ähnlichkeit zu Quantifizieren wurde die Binning Methode mit anschließender Crosscorrelation angewandt \cite{nmrbin}. Jeder Peak $j$ des Spektrums setzt sich aus seiner Intensität $I_{j}$ und seiner Verschiebung $\nu_{j}$ zusammen. Zuerst wird für ein gegebenes NMR Spektrum der Peak mit der größten chemischen Verschiebung $\nu_{max}$ und der kleinsten chemischen Verschiebung $\nu_{min}$ bestimmt und eine Bingröße $b$ festgelegt. Der größte Wert $\nu_{max}$ wird dabei aufgerundet und um eine Bingröße $b$ erhöht (Gleichung \ref{binupper}). Der kleinste Wert $\nu_{min}$ wird abgerundet und um eine Bingröße $b$ verringert (Gleichung \ref{binlower}). \begin{equation} \label{binupper} \nu_{max} = ceiling(max) + b \end{equation} @@ -713,7 +747,7 @@ SI_{ij} = \frac{O_{ij}}{\sqrt{O_{ii} \times O_{jj}}} \end{equation} Für alle Moleküle eines aus dem gesamten Derivationgraph ausgewählten Reaktionspfad wurden Literaturspektren recherchiert. - Jedes mit ORCA berechnete $^{13}$C-NMR, wurde mit den Literaturspektren verglichen. Die für ein Literaturspektrum normierten Ähnlichkeitsindices wurden als Wahrscheinlichkeit angenommen, dass beide NMR-Spektren die Gleiche Substanz abbilden. + Jedes mit dem Quantenchemischen Programm berechnete $^{13}$C-NMR, wurde mit den Literaturspektren verglichen. Die für ein Literaturspektrum normierten Ähnlichkeitsindices wurden als Wahrscheinlichkeit angenommen, dass beide NMR-Spektren die Gleiche Substanz abbilden. \section{Gurobipy} Gurobipy \cite{gurobi} ist ein Python basierter ILP-Solver. Zur Bestimmung der Optimalen Parameter wird ein ILP-Baum verwendet. Die bestimmten Wahrscheinlichkeiten wurden mit dem Derivationgraph kombiniert. Darauf basierend wurde Gruobipy verwendet um einen diese Wahrscheinlichkeiten maximierenden Reaktionpfad in dem Derivationgraph zu identifizieren. \section{Petrinetz Zertifikat} @@ -726,24 +760,26 @@ Koffein ist ein dreifach Methyliertes Purin, welches vor allem in Schwarzem Tee und Kaffeebohnen vorkommt. Es wurde erstmals in den 1820 Jahren isoliert. Heute sind Koffeinhaltige Lebensmittel aus dem Alltag nicht mehr wegzudenken, erfüllt aber auch in Zahlreichen Anwendungsfeldern eine signifikante Rolle. In der Natur wird Koffein aus den Nukleotidbasen Adenin und Guanin über die erst Oxidierung zu Xanthosin und anschließende Methylierung der Stickstoffe des Rings hergestellt (Abb.\ref{coffsynth}). Insbesondere die Methylierung erfolgt erst in der 7, dann in der 3 und zuletzt in der 1 Position. Diese geordnete Methylierung erfolgt mit hoher Spezifität und eignet sich so für eine nähere Untersuchung \cite{caffeinesynth}. \begin{figure} [h] \includegraphics[width=\textwidth]{coffeinesynthesis.png} - \caption{Synthese von Koffein in Pflanzen aus den Nukleotiden Adenin und Guanin. Erst werden die Purin Ringstrukturen Oxidiert und nach der Abspaltung der Ribose die Stickstoffe Methyliert. Die Methylierung erfolgt in der 7, 3 und zuletzt der 1 Position \cite{caffeinesynth}. } + \caption{Synthese von Koffein in Pflanzen aus den Nukleotiden Adenin und Guanin. Erst werden die Purin Ringstrukturen Oxidiert und nach der Abspaltung der Ribose die Stickstoffe methyliert. Die Methylierung erfolgt in der 7, 3 und zuletzt der 1 Position \cite{caffeinesynth}. } \label{coffsynth} \end{figure} \subsection{Vanillin und 3,4-Dihydroxyaldehyd} - Vanillin ist die einer der beliebtesten Aromatischen Moleküle mit hoher Verwendung in Lebensmitteln, wobei der überwiegende Teil synthetisch hergestellt wird. In der Natur wird Vanillin in Vanille Orchideen aus Phenylalanin synthetisiert. Zuerst wird dabei der Aminrest in einer Eliminierung Reaktion zu Zimtsäure umgewandelt. Die Zimtsäure wird dann in der 3 und 4 Position des Phenylrests Hydroxiliert und zu einem Aldehyd oxidiert (Abb. \ref{vansynth}). Die Hydroxylierung und oxidation zu einem Aldehyd eignet sich dabei für eine nähere Untersuchung \cite{vanillinesynth}. + Vanillin ist die einer der beliebtesten Aromatischen Moleküle mit hoher Verwendung in Lebensmitteln, wobei der überwiegende Teil synthetisch hergestellt wird. In der Natur wird Vanillin in Vanille Orchideen aus Phenylalanin synthetisiert. Zuerst wird dabei der Aminrest in einer Eliminierung Reaktion zu Zimtsäure umgewandelt. Die Zimtsäure wird dann in der 3 und 4 Position des Phenylrests Hydroxiliert und zu einem Aldehyd oxidiert (Abb. \ref{vansynth}). Die Hydroxylierung und die Oxidation zu einem Aldehyd eignet sich dabei für eine nähere Untersuchung \cite{vanillinesynth}. \begin{figure} [h] - \includegraphics[width=\textwidth]{vanillsynth.png} + \includegraphics[width=0.9\textwidth]{vanillsynth.png} \caption{Synthese von Vanilline in der Vanille Orchidee. Die Synthese erfolgt aus der Aminosäure Phenylalanin. Dabei wird zuerst die Aminogruppe eliminiert, anschließend der Phenylrest hydroxyliert und die aus der Eliminierung entstandene Doppelbindung oxidiert (rot). Der letzte Schritt ist die Methylierung des 4-Hydroxyrests \cite{vanillinesynth}. } \label{vansynth} \end{figure} \section{Graptransformation: Ein-Molekül-Reaktionen} Für die Ein-Molekül-Reaktionen wurden zuerst in dem Graptransformationstool Transformationsregeln definiert. Diese Regeln wurden dann auf ein Startmolekül angewandt, welches Teil des natürlichen Syntheseprozesses ist. Der betrachtete Syntheseausschnitt wurde dabei mit möglichst wenigen und möglichst einfachen Regen dargestellt. \subsection{Koffein} - Für die Synthese von Koffein wurde mit dem Purin Ring Xanthin gestartet (Abb. \ref{xanthine}) + Für die Synthese von Koffein wurde mit dem Purin Ring Xanthin gestartet (Abb. \ref{xanthine}). \begin{figure} [h] - \includegraphics[width=\textwidth]{xanthine.png} - \caption{Darstellung von Xanthin in dem Graptransformationstool.} - \label{xanthine} + \begin{center} + \includegraphics[width=0.3\textwidth]{xanthine.png} + \caption{Darstellung von Xanthin in dem Graptransformationstool.} + \label{xanthine} + \end{center} \end{figure} Ebenso wurde für die Transformationsregel zum Austausch eines an einen Stickstoff gebundenen Wasserstoff, durch eine Methylgruppe definiert. (Abb. \ref{nmeth}). @@ -761,7 +797,7 @@ \item $p_{0,4}$: 1,7-Dimethylxanthin oder Paraxanthin \item $p_{0,5}$: 3,7-Dimethylxanthin oder Theobromin \end{itemize} - \begin{figure} [h] + \begin{figure} [p] \includegraphics[width=\textwidth]{coffsynthmod.png} \caption{Darstellung aller Synthesepfade von Koffein aus Xanthin in dem Graptransformationstool. Die Graphen $p_{0,0}$ bis $p_{0,5}$ stellen dabei die Zwischenprodukte 1-Methylxanthin, 3-Methylxanthin, 7-Methylxanthin, 1,3-Dimethylxanthin oder Theophylline, 1,7-Dimethylxanthin oder Paraxanthin und 3,7-Dimethylxanthin oder Theobromin dar.} \label{coffsynthmod} @@ -769,10 +805,14 @@ \subsection{Vanillin und 3,4-Dihydroxyaldehyd} Für die Synthese von Vanillin wurde mit Zimtsäure gestartet (Abb. \ref{zimt}). Das natürliche Produkt ist dabei E-Zimtsäure. \begin{figure} [h] - \includegraphics[width=\textwidth]{zimt.png} - \caption{Darstellung von Zimtsäure in dem Graptransformationstool.} - \label{zimt} + \begin{center} + \includegraphics[width=0.3\textwidth]{zimt.png} + \caption{Darstellung von Zimtsäure in dem Graptransformationstool.} + \label{zimt} + \end{center} \end{figure} + + Zur Umsetzung der Zimtsäure zu dem Vanillin Zwischenprodukts, 3,4-Dihydroxybenzaldehyd, wurde eine Regel zur Hydroxylierung der aromatischen Kohlenstoffe (Abb. \ref{hydrox}) und zur Oxidierung einer Doppelbindung mit Carboxylgruppe zu einem Aldehyd (Abb. \ref{aldhyd}) definiert. \begin{figure} [h] \includegraphics[width=\textwidth]{hydrox.png} @@ -780,9 +820,11 @@ \label{hydrox} \end{figure} \begin{figure} [h] - \includegraphics[width=\textwidth]{aldehyd.png} - \caption{Darstellung der Regel zum oxidieren der Zimtsäure Doppelbindung zu einem Aldehyd in dem Graptransformationstool.} - \label{aldhyd} + \begin{center} + \includegraphics[width=0.5\textwidth]{aldehyd.png} + \caption{Darstellung der Regel zum oxidieren der Zimtsäure Doppelbindung zu einem Aldehyd in dem Graptransformationstool.} + \label{aldhyd} + \end{center} \end{figure} Durch das wiederholte anwenden beider Regeln auf Zimtsäure konnte ein Reaktionsnetzerk entwickelt werden, an dessen Ende die Synthese von 3,4-Dihydroxybenzaldehyd steht (Abb. \ref{vanisynthmod}). Die breite Regelanwendung bedeutet die Ermittlung vieler Moleküle, welche nicht mehr zu dem Zielmolekül umgesetzt werden können. Darum wurden die Zwischenprodukte auf die Moleküle beschränkt, die tatsächlich Zwischenprodukte darstellen. Dabei wurden die folgenden Zwischenprodukte bestimmt: \begin{itemize} @@ -793,21 +835,21 @@ \item $p_{0,16}$: 3-Hydroxybenzaldehyd \item $p_{0,17}$: 4-Hydroxybenzaldehyd \end{itemize} - \begin{figure} [h] + \begin{figure} [p] \includegraphics[width=\textwidth]{vanisynthmod.png} \caption{Darstellung aller Synthesepfade von 3,4-Dihydroxybenzaldehyd aus Zimtsäure in dem Graptransformationstool. Nur ein Teil aller Zwischenprodukte wird dabei tatsächlich zu dem gewünschten Produkt.} \label{vanisynthmod} \end{figure} \section{NMR: Ein-Molekül-Reaktionen} - Für alle Zwischenprodukte wurde mit ORCA ein $^{13}$C-NMR berechnet und ein dazugehöriges Literaturspektrum recherchiert. + Für alle Zwischenprodukte wurde mit dem Quantenchemischen Tool ein $^{13}$C-NMR berechnet und ein dazugehöriges Literaturspektrum recherchiert. \subsection{Koffein} - Für alle Xanthinringe lässt sich sagen, dass ausschließlich die Protonen der Methygruppen chemisch Äquivalent zueinander sind. In einem $^{13}$C-NMR weisen also alle Kohlenstoffe ein eigenes Signal mit Intensität 1 auf. Die von ORCA berechneten NMR Spektren wurden den recherchierten Literaturspektren gegenübergestellt (Tabellen \ref{tabelxanthin},\ref{tabel1xanthin},\ref{tabel3xanthin},\ref{tabel7xanthin},\ref{tabel13xanthin},\ref{tabel17xanthin},\ref{tabel37xanthin},\ref{tabel137xanthin}) und ihre Verschiebung zueinander bestimmt. + Für alle Xanthinringe lässt sich sagen, dass ausschließlich die Protonen der Methygruppen chemisch Äquivalent zueinander sind. In einem $^{13}$C-NMR weisen also alle Kohlenstoffe ein eigenes Signal mit Intensität 1 auf. Die mit dem Quantenchemischen Tool berechneten NMR Spektren wurden den recherchierten Literaturspektren gegenübergestellt (Tabellen \ref{tabelxanthin},\ref{tabel1xanthin},\ref{tabel3xanthin},\ref{tabel7xanthin},\ref{tabel13xanthin},\ref{tabel17xanthin},\ref{tabel37xanthin},\ref{tabel137xanthin}) und ihre Verschiebung zueinander bestimmt. \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Xanthin mit einem Literatur Spektrum \cite{xanthinnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.14 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Xanthin mit einem Literatur Spektrum \cite{xanthinnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.14 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabelxanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 112.57 & 108.8 & 3.77 \\ 138.61 & 137.2 & 1.413 \\ @@ -820,11 +862,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 1-Methylxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.39 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 1-Methylxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.39 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel1xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 30.18 & 27 & 3.18 \\ 112.28 & 106.4 & 5.88 \\ @@ -838,11 +880,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 3-Methylxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.35 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 3-Methylxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.35 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel3xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 31.34 & 28.8 & 2.54 \\ 112.87 & 106.9 & 5.97 \\ @@ -856,11 +898,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 7-Methylxanthin mit einem Literatur Spektrum \cite{7xanthinnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.73 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 7-Methylxanthin mit einem Literatur Spektrum \cite{7xanthinnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.73 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel7xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 36.69 & 33.03 & 3.66 \\ 113.78 & 106.9 & 6.88 \\ @@ -874,11 +916,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Theophyllin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.61 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Theophyllin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.61 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel13xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 29.23 & 27.7 & 1.53 \\ 32.05 & 29.7 & 2.35 \\ @@ -893,11 +935,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Paraxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.19 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Paraxanthin mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.19 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel17xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 28.59 & 26.7 & 1.89 \\ 36.8 & 32.9 & 3.9 \\ @@ -912,11 +954,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Theobromin mit einem Literatur Spektrum \cite{theobrominnoMenmr}. Die Methylsignale (ca. 30 ppm) wurden aus einem anderen Spektrum genommen, da diese Angabe fehlte \cite{theobrominnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.63 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Theobromin mit einem Literatur Spektrum \cite{theobrominnoMenmr}. Die Methylsignale (ca. 30 ppm) wurden aus einem anderen Spektrum genommen, da diese Angabe fehlte \cite{theobrominnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.63 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel37xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 30.96 & 29.3 & 1.66 \\ 36.7 & 33.9 & 2.8 \\ @@ -931,11 +973,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Koffein mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.77 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Koffein mit einem Literatur Spektrum \cite{manyxanthinesnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.77 ppm.} \begin{center} \begin{tabular}{ |c|c|c| } \label{tabel137xanthin} - ORCA & Exp & Differenz ORCA - Exp\\ + Berechnet & Exp & Differenz: Berechnet - Exp\\ \hline 28.8 & 27.5 & 1.3 \\ 31.72 & 29.3 & 2.42 \\ @@ -951,15 +993,15 @@ \end{center} \end{table} \newline - Die Methylwasserstoff lassen sich dabei den Signalen um ca. 30 ppm zuordnen, wobei das 1-Methyl Signal mit 28.6 bis 30.18 bei ORCA und 26.7 bis 27.7 in den experimentellen Spektren den niedrigsten Wert aufweist. Die mittlere Verschiebung weißt das 3-Methylsignal mit 31.0 bis 32.1 in ORCA und 28.8 bis 29.7 in den experimentellen Spektren auf. Die größte Verschiebung ist dem 7-Methylsignal mit 36.7 bis 36.9 in ORCA und 32.9 bis 33.9 in den experimentellen Spektren zuzuordnen. Die Signale des Purinrings sind für den größten Teil konstant über alle Moleküle, wobei Xanthin mit 151.03 in ORCA zu 140.5 im Experiment eine besonders große Differenz aufweist. Die größten Unterschiede sind über alle Xanthine bei dem Kohlenstoff neben dem 7-Stickstoff. Über alle Moleküle gemittelt lässt sich bestimmen, dass die von ORCA ermittelten Spektren im Durchschnitt um 2.5 ppm nach oben verschoben sind. + Die Methylwasserstoff lassen sich dabei den Signalen um ca. 30 ppm zuordnen, wobei das 1-Methyl Signal mit 28.6 bis 30.18 bei dem mit dem Quantenchemischen Tool berechneten und 26.7 bis 27.7 in den experimentellen Spektren den niedrigsten Wert aufweist. Die mittlere Verschiebung weißt das 3-Methylsignal mit 31.0 bis 32.1 bei dem mit dem Quantenchemischen Tool berechneten und 28.8 bis 29.7 in den experimentellen Spektren auf. Die größte Verschiebung ist dem 7-Methylsignal mit 36.7 bis 36.9 bei dem mit dem Quantenchemischen Tool berechneten und 32.9 bis 33.9 in den experimentellen Spektren zuzuordnen. Die Signale des Purinrings sind für den größten Teil konstant über alle Moleküle, wobei Xanthin mit 151.03 bei dem mit dem Quantenchemischen Tool berechneten, zu 140.5 im Experiment eine besonders große Differenz aufweist. Die größten Unterschiede sind über alle Xanthine bei dem Kohlenstoff neben dem 7-Stickstoff. Über alle Moleküle gemittelt lässt sich bestimmen, dass die mit dem Quantenchemischen Tool berechneten Spektren im Durchschnitt um 2.5 ppm nach oben verschoben sind. \subsection{Vanillin und 3,4-Dihydroxyaldehyd} - Für 3-hydroxylierte Zwischenprodukte gilt, dass keine Kerne chemisch Äquivalent zueinander sind. Wenn nicht oder nur in der 4-Position hydroxyliert ist, sind jeweils die im Phenylrest gegenüberliegenden Wasserstoffe und Kohlenstoff zueinander chemisch Äquivalent. In einem $^{13}$C-NMR weisen also alle Kohlenstoffe in 3-hydroxilierten Moleküle ein eigenes Signal mit Intensität 1 auf. In nicht oder 4-hydroxylierten Molekülen verschmelzen jeweils zwei Signale zu insgesamt zwei Signalen mit Intensität 2. Die von ORCA berechneten NMR Spektren wurden den recherchierten Literaturspektren gegenübergestellt (Tabellen \ref{tabelzimt},\ref{tabelmcoum},\ref{tabelpcoum},\ref{tabelald},\ref{tabelcafac},\ref{tabel3ald},\ref{tabel4ald},\ref{tabel34ald}) und ihre Verschiebung zueinander bestimmt. + Für 3-hydroxylierte Zwischenprodukte gilt, dass keine Kerne chemisch Äquivalent zueinander sind. Wenn nicht oder nur in der 4-Position hydroxyliert ist, sind jeweils die im Phenylrest gegenüberliegenden Wasserstoffe und Kohlenstoff zueinander chemisch Äquivalent. In einem $^{13}$C-NMR weisen also alle Kohlenstoffe in 3-hydroxilierten Moleküle ein eigenes Signal mit Intensität 1 auf. In nicht oder 4-hydroxylierten Molekülen verschmelzen jeweils zwei Signale zu insgesamt zwei Signalen mit Intensität 2. Die mit dem Quantenchemischen Tool berechneten NMR Spektren wurden den recherchierten Literaturspektren gegenübergestellt (Tabellen \ref{tabelzimt},\ref{tabelmcoum},\ref{tabelpcoum},\ref{tabelald},\ref{tabelcafac},\ref{tabel3ald},\ref{tabel4ald},\ref{tabel34ald}) und ihre Verschiebung zueinander bestimmt. \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Zimtsäure mit einem Literatur Spektrum \cite{cinamnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.02 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Zimtsäure mit einem Literatur Spektrum \cite{cinamnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.02 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabelzimt} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 117.33 & 120.33 & 3 \\ 2 & 128.39 & 133.48 & 5.09 \\ @@ -974,11 +1016,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für m-Coumarsäure mit einem Literatur Spektrum \cite{mcoumnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.53 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für m-Coumarsäure mit einem Literatur Spektrum \cite{mcoumnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.53 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabelmcoum} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 115.3 & 118.6 & 3.3 \\ 1 & 118.6 & 121.09 & 2.49 \\ @@ -995,11 +1037,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für p-Coumarsäure mit einem Literatur Spektrum \cite{pcoumnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.71 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für p-Coumarsäure mit einem Literatur Spektrum \cite{pcoumnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.71 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabelpcoum} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 115.41 & 117.18 & 1.77 \\ 2 & 115.83 & 118.65 & 2.82 \\ @@ -1014,11 +1056,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Benzaldehyd mit einem Literatur Spektrum \cite{aldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.80 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Benzaldehyd mit einem Literatur Spektrum \cite{aldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 4.80 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabelald} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 2 & 128.9 & 133.45 & 4.55 \\ 2 & 129.5 & 135.86 & 6.36 \\ @@ -1031,11 +1073,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für Kaffesäure mit einem Literatur Spektrum \cite{caffacdnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.18 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für Kaffesäure mit einem Literatur Spektrum \cite{caffacdnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 2.18 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabelcafac} - Heigt & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 147.9 & 155.79 & 7.89 \\ 1 & 146.5 & 149.88 & 3.38 \\ @@ -1052,11 +1094,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 3-Hydroxybenzaldehyd mit einem Literatur Spektrum \cite{mhydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.83 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 3-Hydroxybenzaldehyd mit einem Literatur Spektrum \cite{mhydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.83 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabel3ald} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 115 & 122.95 & 7.95 \\ 1 & 122 & 123.33 & 1.33 \\ @@ -1071,11 +1113,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 4-Hydroxybenzaldehyd mit einem Literatur Spektrum \cite{phydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.35 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 4-Hydroxybenzaldehyd mit einem Literatur Spektrum \cite{phydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt 3.35 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabel4ald} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 2 & 116.5 & 118.46 & 1.96 \\ 1 & 130.3 & 135.08 & 4.78 \\ @@ -1088,11 +1130,11 @@ \end{center} \end{table} \begin{table}[htb] - \caption{Vergleich des von ORCA berechneten Spektrum für 3,4-Dihydroxybenzaldehyd mit einem Literatur Spektrum \cite{mphydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt -3.81 ppm.} + \caption{Vergleich des mit dem Quantenchemischen Tool berechneten Spektrum für 3,4-Dihydroxybenzaldehyd mit einem Literatur Spektrum \cite{mphydaldhnmr}. Die Werte sind in ppm angegeben. Die durchschnittliche Differenz beträgt -3.81 ppm.} \begin{center} \begin{tabular}{ |c|c|c|c| } \label{tabel34ald} - Height & Exp & ORCA & Differenz ORCA - Exp\\ + Height & Exp & Berechnet & Differenz: Berechnet - Exp\\ \hline 1 & 113.1 & 114.22 & 1.12 \\ 1 & 117.79 & 115.21 & -2.58 \\ @@ -1107,14 +1149,14 @@ \end{center} \end{table} \newline - Bei den Zwischenprodukten der 3,4-Dihydroxybenzaldehyd Synthese lässt sich im Vergleich zu den Koffein Synthese Zwischenprodukten weniger ein Muster erkennen. Das ist unter anderem darauf zurückzuführen, dass der deutliche Elektronegativitäten Unterschied zwischen Sauerstoff und Wasserstoff einen großen Einfluss auf das Ringsystem erwirkt. Dadurch sind die Signale des Kerngerüsts deutlich weniger Konstant. Das Endprodukt 3,4-Dihydroxybenzaldehyd sticht dabei aber trotzdem heraus, da es im Gegensatz zu allen anderen Spektren durchschnittlich eine größere chemische Verschiebung aufweist. Über alle Spektren gemittelt haben die ORCA Spektren trotzdem eine um 2.8 ppm größere chemische Verschiebung. + Bei den Zwischenprodukten der 3,4-Dihydroxybenzaldehyd Synthese lässt sich im Vergleich zu den Koffein Synthese Zwischenprodukten weniger ein Muster erkennen. Das ist unter anderem darauf zurückzuführen, dass der deutliche Elektronegativitäten Unterschied zwischen Sauerstoff und Wasserstoff einen großen Einfluss auf das Ringsystem erwirkt. Dadurch sind die Signale des Kerngerüsts deutlich weniger Konstant. Das Endprodukt 3,4-Dihydroxybenzaldehyd sticht dabei aber trotzdem heraus, da es im Gegensatz zu allen anderen Spektren durchschnittlich eine größere chemische Verschiebung aufweist. Über alle Spektren gemittelt haben die mit dem Quantenchemischen Tool berechneten Spektren trotzdem eine um 2.8 ppm größere chemische Verschiebung. \section{NMR SI: Ein-Molekül-Reaktionen} - In bisherigen Analysen zu der Genauigkeit von berechneten NMR-Spektren im Vergleich zu Experimentellen Spektren wurde festgestellt, dass einfache DFT Methoden die Effekte von schweren Atomen wie dem in TMS enthaltenden Silizium nicht akkurat bestimmen können. Insbesondere kann davon ausgegangen werden, dass die Frequenz des TMS-Kohenstoff zu gering ausfällt \cite{heavyateff1,heavyatef2}. Das führt wiederum dazu, dass die chemische Verschiebung der Signale im ORCA Spektrum zu hoch ausfällt. Dieser Wert ist systematisch, weshalb er als ungefähres Mittel der Unterschiede zwischen den von ORCA berechneten und experimentellen Spektren quantifiziert wurde. Auf alle Peaks der experimentellen Spektren wurden 2.5 ppm hinzuaddiert. Die Bingröße $b$ variiert in Literaturangaben zwischen 1 und 0.1 ppm \cite{nmrbin,nmrbinsize} mit einer Genauigkeit von 0.1 ppm. Deshalb wurde die Bingröße $b$ (Gleichung \ref{binsize}) variiert und der resultierende Ähnlichkeitsindex $SI$ über alle sinnvollen Werte gemittelt. + In bisherigen Analysen zu der Genauigkeit von berechneten NMR-Spektren im Vergleich zu Experimentellen Spektren wurde festgestellt, dass einfache DFT Methoden die Effekte von schweren Atomen wie dem in TMS enthaltenden Silizium nicht akkurat bestimmen können. Insbesondere kann davon ausgegangen werden, dass die Frequenz des TMS-Kohenstoff zu gering ausfällt \cite{heavyateff1,heavyatef2}. Das führt wiederum dazu, dass die chemische Verschiebung der Signale im mit dem Quantenchemischen Tool berechneten Spektrum zu hoch ausfällt. Dieser Wert ist systematisch, weshalb er als ungefähres Mittel der Unterschiede zwischen den mit dem Quantenchemischen Tool berechneten und experimentellen Spektren quantifiziert wurde. Auf alle Peaks der experimentellen Spektren wurden 2.5 ppm hinzuaddiert. Die Bingröße $b$ variiert in Literaturangaben zwischen 1 und 0.1 ppm \cite{nmrbin,nmrbinsize} mit einer Genauigkeit von 0.1 ppm. Deshalb wurde die Bingröße $b$ (Gleichung \ref{binsize}) variiert und der resultierende Ähnlichkeitsindex $SI$ über alle sinnvollen Werte gemittelt. \begin{equation} \label{binsize} b \in \{0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0\} \end{equation} \subsection{Koffein} - Den Erwartungen entsprechend weißt das ORCA Spektrum von 7-Methylxanthin eine hohe Ähnlichkeit zu dem experimentellen Spektrum von 7-Methylxanthin auf. Das Spektrum von Paraxanthin ist jedoch noch etwas ähnlicher. Die Spektren von Theobromin haben im Vergleich dazu die größten Übereinstimmungen, wobei Koffein am zweit ähnlichsten ist. Allgemein scheint eine Identifikation des 7-Methylrest gut zu funktionieren, jedoch keine einfache Unterscheidung der Restlichen Methylgruppen möglich zu sein. Da in allen Molekülen das Xanthin-Grundgerüst vorliegt und die Addition einer Methylgruppe dieses nicht zu sehr verändert, haben alle Moleküle eine signifikante Ähnlichkeit zueinander (Tabelle \ref{nmrsimcoff}). + Den Erwartungen entsprechend weißt das mit dem Quantenchemischen Tool berechnete Spektrum von 7-Methylxanthin eine hohe Ähnlichkeit zu dem experimentellen Spektrum von 7-Methylxanthin auf. Das Spektrum von Paraxanthin ist jedoch noch etwas ähnlicher. Die Spektren von Theobromin haben im Vergleich dazu die größten Übereinstimmungen, wobei Koffein am zweit ähnlichsten ist. Allgemein scheint eine Identifikation des 7-Methylrest gut zu funktionieren, jedoch keine einfache Unterscheidung der Restlichen Methylgruppen möglich zu sein. Da in allen Molekülen das Xanthin-Grundgerüst vorliegt und die Addition einer Methylgruppe dieses nicht zu sehr verändert, haben alle Moleküle eine signifikante Ähnlichkeit zueinander (Tabelle \ref{nmrsimcoff}). \begin{table}[htb] \caption{Resultierende normalisierte Wahrscheinlichkeiten beim Vergleich aller Zwischenprodukte der Koffeinsynthese, sowie Xanthin und Koffein mit den natürlichen Zwischenprodukten 7-Methyxanthin und Theobromin.} \begin{center} @@ -1287,7 +1329,7 @@ \end{table} Dabei ist jedoch anzumerken, dass die Lösung des ILP für das erste Moleküle 4-Hydroxybenzaldehyd und für das zweite Molekül p-Coumarsäure gewählt hat. Die Zuordnung erfolgte also genau anders herum. Zudem ist davon auszugehen, dass die zweitbeste Lösung genau den selben Wert Zielwert aufweist. \section{Fazit: Ein-Molekül-Reaktionen} - Bei den bisher betrachteten Ein-Molekül-Reaktionen wurde immer nur ein festgelegtes Startmolekül in das System gegeben. Dieses Startmolekül wurde nach Transformationsregeln variiert, wobei jedoch nach dem natürlichen Vorbild auch genau ein Zielmolekül synthetisiert werden sollte. In dem Koffein Beispiel gab es dabei keine Enantiomere oder E/Z-Isomere. In dem Vanille Beispiel gab es keine Enatiomere. Es gab mit Zimtsäure, Coumarsäure und Kaffesäure zwar E/Z-Isomere, welche aber durch die natürliche Vorgabe von E-Zimtsäure bereits vorgegeben waren. Außerdem entstand keine neue Doppelbindung mit einem E/Z-Isomer durch Graphtransformation. Der Schluss von dem Graphen auf eine Geometrie war deswegen immer eindeutig. \newline Die Berechnung der NMR Spektren war trotzdem fehleranfällig. Dabei konnten bestimmte Molekülveränderungen besser in dem NMR-Berechnungstool abgebildet werden. Eine Methylierung erzeugte dabei nur eine geringe Veränderung im Xanthingrundgerüst, weshalb die Zuordnung vor allem in dem Signal der Methylgruppe lag. Die Hydroxylierung und Oxidierung zum Aldehyd resultierten in deutlichen Veränderungen der Phenylgruppe, weshalb das Grundgerüst selber verändert wurde. \newline Für die Synthesen waren immer genau drei Reaktionen nötig, welche mittels des ILP nur bezüglich ihrer Reihenfolge variiert werden konnte. Das Problem ließe sich daher ebenfalls durch die einfache Addition zweier Moleküle entlang eines ausgewählten Pfades lösen. Der Raum möglicher Lösungen ist mit 6 pro Hypergraph stark begrenzt. Trotzdem eigneten sich beide Beispiele mit der natürlich auftretenden Selektivität der Reihenfolge, der guten Differenzierbarkeit der NMR-Spektren und Kompaktheit der Synthese als Graphtransformationsregeln als Demonstration des Konzeptes. \newline Für ausgewählte Literaturspektren von nicht in der natürlichen Synthese erwarteten Molekülen wurden ebenfalls die Crossskorrelationen mit den berechneten Spektren ermittelt. Dabei konnte ebenfalls eine erhöhte Korrelation mit dem zugehörigen berechneten Spektrum bestimmt werden. Das ILP konnte dabei den neuen Syntheseplan ebenfalls zuverlässig zuordnen. Die Auswahl eines Syntheseplans basierend auf der Ähnlichkeit von NMR-Spektren ist daher gerechtfertigt und stellt eine Verbesserung gegenüber der Auswahl ohne selbige dar. + Bei den bisher betrachteten Ein-Molekül-Reaktionen wurde immer nur ein festgelegtes Startmolekül in das System gegeben. Dieses Startmolekül wurde nach Transformationsregeln variiert, wobei jedoch nach dem natürlichen Vorbild auch genau ein Zielmolekül synthetisiert werden sollte. In dem Koffein Beispiel gab es dabei keine Enantiomere oder E/Z-Isomere. In dem Vanille Beispiel gab es keine Enatiomere. Es gab mit Zimtsäure, Coumarsäure und Kaffesäure zwar E/Z-Isomere, welche aber durch die natürliche Vorgabe von E-Zimtsäure bereits vorgegeben waren. Außerdem entstand keine neue Doppelbindung mit einem E/Z-Isomer durch Graphtransformation. Der Schluss von dem Graphen auf eine Geometrie war deswegen immer eindeutig. \newline Die Berechnung der NMR Spektren war trotzdem fehleranfällig. Dabei konnten bestimmte Molekülveränderungen besser in dem NMR-Berechnungstool abgebildet werden. Eine Methylierung erzeugte dabei nur eine geringe Veränderung im Xanthingrundgerüst, weshalb die Zuordnung vor allem in dem Signal der Methylgruppe lag. Die Hydroxylierung und Oxidierung zum Aldehyd resultierten in deutlichen Veränderungen der Phenylgruppe, weshalb das Grundgerüst selber verändert wurde. \newline Für die Synthesen waren immer genau drei Reaktionen nötig, welche mittels des ILP nur bezüglich ihrer Reihenfolge variiert werden konnte. Das Problem ließe sich daher ebenfalls durch die einfache Addition zweier Moleküle entlang eines ausgewählten Pfades lösen. Der Raum möglicher Lösungen ist mit 6 pro Hypergraph stark begrenzt. Trotzdem eigneten sich beide Beispiele mit der natürlich auftretenden Selektivität der Reihenfolge, der guten Differenzierbarkeit der NMR-Spektren und Kompaktheit der Synthese als Graphtransformationsregeln als Demonstration des Konzeptes. Es ist anzumerken, dass die erwartete Synthese über die Auswahl der Referenzspektren festgelegt wurde. Diese Synthese wurde über NMR-Spektren abstrahiert. Es lässt sich so sagen, dass die NMR-Spektren in dieser Analyse die Struktur hinreichend Codieren, aber nicht eine Unbekannte Synthese vollständig hergeleitet wurde. \newline Für ausgewählte Literaturspektren von nicht in der natürlichen Synthese erwarteten Molekülen wurden ebenfalls die Crossskorrelationen mit den berechneten Spektren ermittelt. Dabei konnte ebenfalls eine erhöhte Korrelation mit dem zugehörigen berechneten Spektrum bestimmt werden. Das ILP konnte dabei den neuen Syntheseplan ebenfalls zuverlässig zuordnen. Die Auswahl eines Syntheseplans basierend auf der Ähnlichkeit von NMR-Spektren ist daher gerechtfertigt und stellt eine Verbesserung gegenüber der Auswahl ohne selbige dar. \section{Multi-Molekül-Reaktionen} Um die Grenzen der Möglichkeiten des ILP weiter auszureizen werden im Folgenden Reaktionen, die ebenfalls mit einfachen Reaktionsregeln ein hochvernetztes Reaktionsnetzwerk erzeugen betrachtet. \section{Olefin Metathese und Diels Alder} @@ -1315,9 +1357,11 @@ \subsection{Olefin Metathese und Diels Alder} In dem Graptransformationstool wurde mit dem Molekül Butadien (Abb. \ref{butadienmod}) gestartet. Auf dieses wurden wiederholt die Olefin Metathese (Abb. \ref{olmetmod}) und die Diels Alder Reaktion (Abb. \ref{dialdmod}) angewendet. \begin{figure} [h] - \includegraphics[width=\textwidth]{butadienmod.png} - \caption{Butadien in dem Graptransformationstool.} - \label{butadienmod} + \begin{center} + \includegraphics[width=0.5\textwidth]{butadienmod.png} + \caption{Butadien in dem Graptransformationstool.} + \label{butadienmod} + \end{center} \end{figure} \begin{figure} [h] \includegraphics[width=\textwidth]{olmetmod.png} @@ -1331,7 +1375,7 @@ \end{figure} Bei dieser Reaktion ist es anders als bei den bisherigen Reaktionen möglich, dass der Ergebnisraum unbegrenzt wachsen kann. Darum sind Beschränkungen des Ergebnisraums nötig. Die einfachste Beschränkung der Ergebnisse ist eine Obergrenze für die Anzahl an Atomen. Damit Butadien als Startmolekül diese Begrenzung erfüllt, müssen mindestens 4 Kohlenstoffe zugelassen werden. Damit die Diels Alder Reaktion stattfinden kann müssen 6 Kohlenstoffe erlaubt sein. Die Regeln zeigen einen diversen Raum an gefundenen Molekülen bei 10 Kohlenstoffen. Da dies die Computerleistung stark beansprucht muss der Raum weiter eingeschränkt werden. Die Olefin Metathese ist bekannt dafür, Ringe mit großer Ringspannung aufzubrechen \cite{olefinmetathese}. Besonders strapaziert sind kleine Ringe mit der Größe 3 und 4, sowie große Ringe. Ein Kohlenstoff Ring der Größe 6 ist am stabilsten \cite{ringstrain}. Da die Olefin Metathese mit hoher Selektivität Ringe mit hoher Spannung aufbricht, ist davon auszugehen, dass zu große und zu kleine Ringe nicht Teil des Ergebnisraums sind. Insbesondere ist nur der 6 Ring als die stabilste Ringgröße zu erwarten. Deshalb wurden für jedes gefundene Molekül alle sehnenlosen Ringe gefunden und alle Ringe, die nicht die Größe 6 hatten aus dem Ergebnis Raum entfernt. Eine weitere Quelle der Ringspannung sind überlappende Ringe. Norbornan wird zum Beispiel aus drei überlagernden Ringen gebildet. Da auch in diesen Molekülen hohe Ringspannung vorliegt wurden alle Moleküle mit Ringen, die mehr als zwei gemeinsame Atome haben aus dem Ergebnisraum entfernt. Die letzte Begrenzung für Ringspannung ist, dass kein Atom in vier Ringen sein kann. \newline Mit der Beschränkung durch wurden durch die Regelanwendung 19 Moleküle mit etwa 200 Transformationen aus Butadien entwickelt. - Die Moleküle und ihre SMILE-Strings lauten: + Die Moleküle und ihre SMILES-Strings lauten: \begin{itemize} \item Butadien: C=CC=C \item Ethylen: C=C @@ -1559,13 +1603,13 @@ \subsubsection{Knoten Auswahl} Beide Lösungen der Knotenauswahlmethode erfüllen ein Petrinetzzertifikat. \section{Fazit: Multi-Molekül-Reaktionen} - Im Vergleich zu einem kleinen Netzwerk mit Festgelegten Start- und Zielmolekülen, ist die Formulierung der Zielfunktionen und Einschränkungen für ein Multi Molekül Netzwerk deutlich komplexer. Dazu kommt die Entscheidung, nur die Ausgangsmoleküle zu definieren. Dabei kommt nur das ILP mit der Kantenwahrscheinlichkeit als Produkt gar nicht auf die erwartete Lösung. In beiden anderen Modellen ist die direkte Synthese von Benzol die erste Lösung mit Petrinetzzertifikat. Das ILP mit der Kantenwahrscheinlichkeit als Durchschnitt hatte trotzdem einige Lösungen, welche deutlich von der erwarteten Lösung abwichen und teilweise keine Kanten mit dieser teilten. Das ILP bei dem drei Knoten ausgewählt wurden, die in der Synthese vorkommen müssen war dabei noch effizienter. Die zweit beste Lösung bei diesem ILP ist ebenfalls eine realistische Möglichkeit unter den Reaktionsbedingungen, wenn gleich sie in der Kohlenstoffeffizienz geringer ist. Die Lösung würde eigentlich vier Butadien zum Start benötigen. Da bei den Reaktionen aber ein neues Butadien entsteht, sind die ILP Bedingungen aber erfüllt. Da Butadien aber als Startmolekül theoretisch unbegrenzt vorliegt, ist die Synthese trotzdem chemisch möglich. Das überschüssige Butadien kann zum Beginn der nächsten Synthese erneute verbraucht werden. Zur Verifizierung des Butadien Beispiels wurden NMR-unabhängige Werte verwendet. Die betrachtete Synthese von Benzol aus Butadien stellt demnach auch ohne die Wahrscheinlichkeiten die optimale Lösung dar, wenn das Zielmolekül festgelegt wird. Ohne Wahrscheinlichkeiten oder mit zufälligen Wahrscheinlichkeiten und einem nicht definierten Zielmolekül, gibt es jedoch entweder eine Lösung ohne Reaktionen oder eine Lösung mit zufälligen Zielmolekül. Auch hier resultiert die Verwendung der NMR-basierten Wahrscheinlichkeiten in einer zielgerichteteren Lösungsauswahl. + Im Vergleich zu einem kleinen Netzwerk mit Festgelegten Start- und Zielmolekülen, ist die Formulierung der Zielfunktionen und Einschränkungen für ein Multi Molekül Netzwerk deutlich komplexer. Dazu kommt die Entscheidung, nur die Ausgangsmoleküle zu definieren. Dabei kommt nur das ILP mit der Kantenwahrscheinlichkeit als Produkt gar nicht auf die erwartete Lösung. In beiden anderen Modellen ist die direkte Synthese von Benzol die erste Lösung mit Petrinetzzertifikat. Das ILP mit der Kantenwahrscheinlichkeit als Durchschnitt hatte trotzdem einige Lösungen, welche deutlich von der erwarteten Lösung abwichen und teilweise keine Kanten mit dieser teilten. Das ILP bei dem drei Knoten ausgewählt wurden, die in der Synthese vorkommen müssen war dabei noch effizienter. Die zweit beste Lösung bei diesem ILP ist ebenfalls eine realistische Möglichkeit unter den Reaktionsbedingungen, wenn gleich sie in der Kohlenstoffeffizienz geringer ist. Die Lösung würde eigentlich vier Butadien zum Start benötigen. Da bei den Reaktionen aber ein neues Butadien entsteht, sind die ILP Bedingungen aber erfüllt. Da Butadien aber als Startmolekül theoretisch unbegrenzt vorliegt, ist die Synthese trotzdem chemisch möglich. Das überschüssige Butadien kann zum Beginn der nächsten Synthese erneute verbraucht werden. Zur Verifizierung des Butadien Beispiels wurden NMR-unabhängige Werte verwendet. Die betrachtete Synthese von Benzol aus Butadien stellt demnach auch ohne die Wahrscheinlichkeiten die optimale Lösung dar, wenn das Zielmolekül festgelegt wird. Ohne Wahrscheinlichkeiten oder mit zufälligen Wahrscheinlichkeiten und einem nicht definierten Zielmolekül, gibt es jedoch entweder eine Lösung ohne Reaktionen oder eine Lösung mit zufälligen Zielmolekül. Auch hier resultiert die Verwendung der NMR-basierten Wahrscheinlichkeiten in einer zielgerichteteren Lösungsauswahl. \newline Auch die Synthese von Benzol aus Butadien zeigt, dass die in den NMR-Spektren enthaltenen Informationen eine Rekonstruktion der vorgegeben Reaktionen ermöglicht. Mehr als in den natürlich Auftretenden Synthesen muss angemerkt werden, dass die durch NMR-Spektren repräsentierten Reaktionen nicht auf in der Literatur vorgefundenen Synthesen oder im Labor gemessenen Spektren basiert. \chapter{Zusammenfassung und Ausblick} - In dieser Masterarbeit wurde die Möglichkeit untersucht die Syntheseplanung und -analyse mittels NMR-Spektren zu automatisieren. Dabei wurden die charakteristischen Verschiebungen in $^{13}$C-NMR-Spektren verwendet, um die Wahrscheinlichkeit einzelner Moleküle und Reaktionen zu bestimmen. Diese Wahrscheinlichkeiten wurden über eine ILP-Berechnung optimiert. Noch öfter als $^{13}$C-NMR-Spektren in der organischen Chemie sind die $^{1}$H-NMR-Spektren. Diese haben zu den charakteristischen Verschiebungen noch zusätzliche Informationen durch Multiplettaufspaltungen. Da Wasserstoff im Gegensatz zu Kohlenstoffen als Protonen abgespalten werden können, kommt es vor allem bei Wasserstoff-Stickstoff und Wasserstoff-Sauerstoff Bindungen zu großen Schwankungen in der chemischen Verschiebung. Hinzu kommt, dass ORCA in der Berechnung der $^{1}$H-NMR-Spektren deutlich inkonstanter von den experimentellen Spektren abweicht. Zudem kommt es bei der Berechnung der Peakintensitäten und Aufspaltung zu größeren Fehlern, weshalb es für die verwendete Analyse nicht geeignet ist. Die Crosskorrelation bietet eine sehr einfache Methode zum Vergleich von NMR-Spektren. Da jedoch bei den $^{1}$H-NMR-Spektren die Multiplettaufspaltung oft mehr Informationen enthält, als nur Intensität und chemische Verschiebung, geht bei der Analyse eine zentrale Komponente verloren. Beim Vergleich zwischen Spektren der gleichen Substanz, ist die Crosskorrelation auch bei $^{1}$H-NMR-Spektren geeignet, da nur leichte Verschiebungen der Peaks zu erwarten sind. Wenn jedoch zwei verschiedene Substanzen verglichen werden, kann die Verschiebung schon größer sein, weshalb die Ähnlichkeit gering ist, auch wenn die Spektren als Ganzes betrachtet ähnlich sind. Für eine solche Analyse könnte ein Machine Learning Model trainiert werden \cite{nmrsimml}, welches diese Details berücksichtigt. Zum Training dieses Models müssten jedoch deutlich mehr Beispiele verwendet werden und der NMR-Vergleich müsste eine deutlich zentralere Rolle in dieser Arbeit einnehmen. Mehr Beispiele können zudem verwendet werden um den Schweratomeffekt in der NMR-Berechnung zu Quantifizieren, sowie allgemeine Fehler in der Verschiebung zu ermitteln und so den idealen Verschiebungswert zu ermitteln. Die Kombination beider Ein-Molekül-Reaktionen legt jedoch nahe, dass dieser Fehler nicht durch eine Verschiebung mit einer Konstante zu beschreiben ist. Die Lösungen des ILP erfüllen die Erwartungen. In der NMR-Spektroskopie ist es auch möglich zwei Substanzen in einem NMR-Spektrum abzubilden. Dabei kann der Vergleich der Intensität der zugeordneten Peaks bestimmt werden, welches Stoffmengenverhältnis beide Substanzen zueinander haben \cite{nmrquant}. Es ist also möglich anstelle von mehreren NMR-Spektren für eine Synthese, nur ein gemeinsames NMR-Spektrum zu bestimmen und auf Basis dieses Spektrums neben den vorliegenden Substanzen, auch deren relative Stoffmenge zu bestimmen. Sowohl die natürlichen Synthesen im Organismus, als auch die Olefin Metathese und Diels Alder Reaktion für Butadien, eignen sich als Reaktion in einem Topf. Dadurch könnten die Startmoleküle mit den Enzymen und Katalysatoren in eine Lösung gebracht werden und nach einer festen Zeit NMR-Spektren aufgenommen werden. Basierend auf diesen Spektren könnten die relativen Stoffmengen und basierend auf diesen die Gleichgewichtskonstanten für diese Reaktionen bestimmt werden. Zudem erlaubt eine solche Analyse die Bestimmung von Nebenprodukten, welche in dem bisherigen Ansatz nicht definiert wurden. Die bisherige Untersuchung eignet sich trotzdem als eine Demonstration der möglichen Kombination beider bisher getrennter Felder. + In dieser Masterarbeit wurde die Möglichkeit untersucht die Syntheseplanung und -analyse mittels NMR-Spektren zu automatisieren. Dabei wurden die charakteristischen Verschiebungen in $^{13}$C-NMR-Spektren verwendet, um die Wahrscheinlichkeit einzelner Moleküle und Reaktionen zu bestimmen. Diese Wahrscheinlichkeiten wurden über eine ILP-Berechnung optimiert. Noch öfter als $^{13}$C-NMR-Spektren in der organischen Chemie sind die $^{1}$H-NMR-Spektren. Diese haben zu den charakteristischen Verschiebungen noch zusätzliche Informationen durch Multiplettaufspaltungen. Da Wasserstoff im Gegensatz zu Kohlenstoffen als Protonen abgespalten werden können, kommt es vor allem bei Wasserstoff-Stickstoff und Wasserstoff-Sauerstoff Bindungen zu großen Schwankungen in der chemischen Verschiebung. Hinzu kommt, dass da Quantenchemischen Tool in der Berechnung der $^{1}$H-NMR-Spektren deutlich inkonstanter von den experimentellen Spektren abweicht. Zudem kommt es bei der Berechnung der Peakintensitäten und Aufspaltung zu größeren Fehlern, weshalb es für die verwendete Analyse nicht geeignet ist. Die Crosskorrelation bietet eine sehr einfache Methode zum Vergleich von NMR-Spektren. Da jedoch bei den $^{1}$H-NMR-Spektren die Multiplettaufspaltung oft mehr Informationen enthält, als nur Intensität und chemische Verschiebung, geht bei der Analyse eine zentrale Komponente verloren. Beim Vergleich zwischen Spektren der gleichen Substanz, ist die Crosskorrelation auch bei $^{1}$H-NMR-Spektren geeignet, da nur leichte Verschiebungen der Peaks zu erwarten sind. Wenn jedoch zwei verschiedene Substanzen verglichen werden, kann die Verschiebung schon größer sein, weshalb die Ähnlichkeit gering ist, auch wenn die Spektren als Ganzes betrachtet ähnlich sind. Für eine solche Analyse könnte ein Machine Learning Model trainiert werden \cite{nmrsimml}, welches diese Details berücksichtigt. Zum Training dieses Models müssten jedoch deutlich mehr Beispiele verwendet werden und der NMR-Vergleich müsste eine deutlich zentralere Rolle in dieser Arbeit einnehmen. Mehr Beispiele können zudem verwendet werden um den Schweratomeffekt in der NMR-Berechnung zu Quantifizieren, sowie allgemeine Fehler in der Verschiebung zu ermitteln und so den idealen Verschiebungswert zu ermitteln. Die Kombination beider Ein-Molekül-Reaktionen legt jedoch nahe, dass dieser Fehler nicht durch eine Verschiebung mit einer Konstante zu beschreiben ist. Die Lösungen des ILP erfüllen die Erwartungen. In der NMR-Spektroskopie ist es auch möglich zwei Substanzen in einem NMR-Spektrum abzubilden. Dabei kann der Vergleich der Intensität der zugeordneten Peaks bestimmt werden, welches Stoffmengenverhältnis beide Substanzen zueinander haben \cite{nmrquant}. Es ist also möglich anstelle von mehreren NMR-Spektren für eine Synthese, nur ein gemeinsames NMR-Spektrum zu bestimmen und auf Basis dieses Spektrums neben den vorliegenden Substanzen, auch deren relative Stoffmenge zu bestimmen. Sowohl die natürlichen Synthesen im Organismus, als auch die Olefin Metathese und Diels Alder Reaktion für Butadien, eignen sich als Reaktion in einem Topf. Dadurch könnten die Startmoleküle mit den Enzymen und Katalysatoren in eine Lösung gebracht werden und nach einer festen Zeit NMR-Spektren aufgenommen werden. Basierend auf diesen Spektren könnten die relativen Stoffmengen und basierend auf diesen die Gleichgewichtskonstanten für diese Reaktionen bestimmt werden. Zudem erlaubt eine solche Analyse die Bestimmung von Nebenprodukten, welche in dem bisherigen Ansatz nicht definiert wurden. Die bisherige Untersuchung eignet sich trotzdem als eine Demonstration der möglichen Kombination beider bisher getrennter Felder. \chapter{Danksagung} - + Ich möchte die Gelegenheit nutzen, mich herzlichst bei dem Arbeitskreis Chemieinformatik zu bedanken. Besonderer Dank gilt Daniel Merkle, der mcih sowohl tatkräftig bei dem Inhaltlichen unterstützt hat als auch durch seine große Begeisterung eine konstante Quelle der Motivation war. Ebenso danke ich Yuri Kolcak, Addie Jordon und Cassandra König für die beratende Expertise zu theoretischen und inhaltlichen Fragen. Auch Marcel Friedrichs hat mir besonders bei technischen Problemen unterstützt. Zuletzt danke ich Verena Uhlig und Nicole Schellenberg, für die organisatorischen Unterstützung und das sie Daniel erinnert haben, wenn meine Fragen in den vielen Aufgaben etwas untergegangen sind. %%================================================================================== \addcontentsline{toc}{chapter}{Quellenverzeichnis} \renewcommand\bibname{Quellenverzeichnis} diff --git a/Report/refs.bib b/Report/refs.bib index 3c51870..da19859 100644 --- a/Report/refs.bib +++ b/Report/refs.bib @@ -24,10 +24,6 @@ url = {https://doi.org/10.1063/5.0004608}, eprint = {https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/5.0004608/16740678/224108_1_online.pdf}, } -@misc{ Nobody06, - author = "Nobody Jr", - title = "My Article", - year = "2006" } @book{bender2006foundations, title={Foundations of Combinatorics with Applications}, @@ -40,8 +36,7 @@ isbn={978-0486446035}, note={ISBN-10: 0-486-44603-4} } -@book{ - Graphtheory, +@book{Graphtheory, title = {Graphentheorie : eine anwendungsorientierte Einführung}, series = {Mathematik-Studienhilfen}, author = {Tittmann, Peter}, @@ -109,7 +104,7 @@ eprint = {https://pubs.acs.org/jceda8/article-pdf/68/6/456/416109/ed068p456.pdf}, } @article{hypergraphpath, - author = {Spencer Krieger and John Kececioglu}, + author = {Krieger, Spencer and Kececioglu, John}, title ={Shortest Hyperpaths in Directed Hypergraphs for Reaction Pathway Inference}, journal = {Journal of Computational Biology}, @@ -153,6 +148,7 @@ adsnote = {Provided by the SAO/NASA Astrophysics Data System} } @inbook{ilp, + author = {Chen, Der-San and Batson, Robert G. and Dang, Yu}, publisher = {John Wiley and Sons, Ltd}, isbn = {9781118166000}, title = {Linear Programming—Fundamentals}, @@ -180,6 +176,14 @@ pages = {223–252}, numpages = {30} } +@phdthesis{petri1962kommunikation, + author = {Petri, Carl Adam}, + title = {Kommunikation mit Automaten}, + school = {Technische Universit{"a}t Darmstadt}, + year = {1962}, + address = {Darmstadt, Germany}, + type = {Dissertation} +} @book{atkinsdft, abstract = {This text unravels those fundamental physical principles which explain how all matter behaves. It takes us from the foundations of quantum mechanics, through quantum models of atomic, molecular, and electronic structure, and on to discussions of spectroscopy, and the electronic and magnetic properties of molecules.}, author = {Atkins, P. W. and Friedman, R. S.}, @@ -532,26 +536,20 @@ pages = {46}, keywords = {Schiff base, Spectral studies, Computational studies, Energy gap, Refractive index.}, url = {https://papers.ssrn.com/sol3/papers.cfm?abstract_id=4934411}, - eprint = {https://onlinelibrary.wiley.com/doi/pdf/10.1002/app.23537}, - abstract = {Optical materials organic in nature are leading materials exhibiting semiconducting properties is trend of present technology in optical and electronic applications. Active organic materials of Schiff bases are of vital importance in terms of their molecular properties, band gap, refractive index and dielectric operated at room temperature than compared to inorganic materials at elevated temperatures during synthesis. The present article focuses on the development of thin films with the synthesis of Schiff base of 4-hydroxy benzaldehydes and substituted anilines using the green synthesis method. The formation of the Schiff base compounds was confirmed with spectroscopic methods with shifts in wavenumbers in infrared spectra, transition with optical band gap with ultraviolet spectra and chemical environment with chemical shifts using proton NMR. Powdered XRD provide information of structure, composition and crystalline proximity of the synthesized Schiff base compounds. Optical properties refractive index and dielectric constant were attributed with spectroscopic ellipsometer. Computational studies were performed using the Gaussian 16 package with the B3LYP method basis set 6-311++** for all molecular compounds to confirm the molecular structures, optimized geometry, and electronic and optical properties. The insights of these properties are best visualized in terms of quantum mechanical descriptors responsible due to changes in electron density. Studies of these Schiff base compounds with nitro groups proved to exhibit optical properties and as an excellent organic semiconducting material with an energy gap of 3.08 eV; refractive index of 2.074, and dielectric constant of 4.303. }, + abstract = {Optical materials organic in nature are leading materials exhibiting semiconducting properties is trend of present technology in optical and electronic applications. Active organic materials of Schiff bases are of vital importance in terms of their molecular properties, band gap, refractive index and dielectric operated at room temperature than compared to inorganic materials at elevated temperatures during synthesis. The present article focuses on the development of thin films with the synthesis of Schiff base of 4-hydroxy benzaldehydes and substituted anilines using the green synthesis method. The formation of the Schiff base compounds was confirmed with spectroscopic methods with shifts in wavenumbers in infrared spectra, transition with optical band gap with ultraviolet spectra and chemical environment with chemical shifts using proton NMR. Powdered XRD provide information of structure, composition and crystalline proximity of the synthesized Schiff base compounds. Optical properties refractive index and dielectric constant were attributed with spectroscopic ellipsometer. Computational studies were performed using the Gaussian 16 package with the B3LYP method basis set 6-311++ for all molecular compounds to confirm the molecular structures, optimized geometry, and electronic and optical properties. The insights of these properties are best visualized in terms of quantum mechanical descriptors responsible due to changes in electron density. Studies of these Schiff base compounds with nitro groups proved to exhibit optical properties and as an excellent organic semiconducting material with an energy gap of 3.08 eV; refractive index of 2.074, and dielectric constant of 4.303. }, year = {2024} } @article{mphydaldhnmr, - author = {Syfani, Nova and Putra, Deddi Prima and Arbani, Dayar}, - title = {3,4-DIHYDROXYBENZOIC ACID AND 3,4-DIHYDROXYBENZALDEHYDE FROM THE FERN - Trichomanes chinense L.; ISOLATION, ANTIMICROBIAL AND ANTIOXIDANT PROPERTIES}, - journal = {Indo. J. Chem.,}, + author = {Nova Syafni and Deddi Putra and Dayar Arbain}, + title = {3,4-DIHYDROXYBENZOIC ACID AND 3,4-DIHYDROXYBENZALDEHYDE FROM THE FERN Trichomanes chinense L.; ISOLATION, ANTIMICROBIAL AND ANTIOXIDANT PROPERTIES}, + journal = {Indonesian Journal of Chemistry}, volume = {12}, number = {3}, - pages = {273-278}, - keywords = {Trichomanes chinense L.; 3,4-dihydroxybenzoic acid; 3,4-dihydroxybenzaldehyde; antioxidant; - antimicrobial}, - url = {https://academia-edu-documents.ada3b51d29be5ae5c31d26340608fd48.r2.cloudflarestorage.com/76337429/62cb66d00830376d6243dfc70e9c9c13f07a-libre.pdf?response-content-disposition=inline%3B%20filename%3D3_4_DIHYDROXYBENZOIC_ACID_AND_3_4_DIHYDR.pdf&response-content-type=application%2Fpdf&X-Amz-Algorithm=AWS4-HMAC-SHA256&X-Amz-Credential=62bb68dcc7da7de029ac4fdac624cee9%2F20261018%2Fauto%2Fs3%2Faws4_request&X-Amz-Date=20261018T014804Z&X-Amz-Expires=3600&X-Amz-SignedHeaders=host&X-Amz-Signature=2d857d9fd2556313a486db1447aa14a97dca8a72ac8aa120ff8d3c255860bd06}, - abstract = {3,4-dihydroxybenzoic acid (1) and 3,4-dihydroxybenzaldehyde (2) have been isolated from ethyl acetate - fraction of methanolic fractions of leaves, stems and roots of the fern Trichomanes chinense L. (Hymenophyllaceae). - These two compounds also showed significant antioxidant using DPPH and antimicrobial activities using the disc - diffusion assay.}, - year = {2012} + year = {2012}, + keywords = {Trichomanes chinense L.; 3,4-dihydroxybenzoic acid; 3,4-dihydroxybenzaldehyde; antioxidant; antimicrobial}, + abstract = {3,4-dihydroxybenzoic acid (1) and 3,4-dihydroxybenzaldehyde (2) have been isolated from ethyl acetate fraction of methanolic fractions of leaves, stems and roots of the fern Trichomanes chinense L. (Hymenophyllaceae). These two compounds also showed significant antioxidant using DPPH and antimicrobial activities using the disc diffusion assay.}, + issn = {2460-1578}, pages = {273--278}, doi = {10.22146/ijc.21342}, + url = {https://journal.ugm.ac.id/ijc/article/view/21342} } @article{heavyateff1, author = {Lodewyk, Michael W. and Siebert, Matthew R. and Tantillo, Dean J.}, @@ -630,7 +628,7 @@ doi = {https://doi.org/10.1002/anie.198603121}, url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.198603121}, eprint = {https://onlinelibrary.wiley.com/doi/pdf/10.1002/anie.198603121}, - abstract = {Abstract “Die Ringschließung ist offenbar diejenige Erscheinung, welche am meisten über die räumliche Anordnung der Atome Auskunft geben kann. Wenn eine Kette von 5 und 6 Gliedern sich leicht, eine von weniger oder mehr Gliedern sich schwierig oder auch gar nicht schließen läßt, so müssen dafür offenbar räumliche Gründe vorhanden sein.… Die vier Valenzen des Kohlenstoffatoms wirken in den Richtungen, welche den Mittelpunkt der Kugel mit den Tetraederecken verbinden, und welche miteinander einen Winkel von 109°28′ machen. Die Richtung der Anziehung kann eine Ablenkung erfahren, die jedoch eine mit der Größe der Letzteren wachsende Spannung zur Folge hat,”[ Ring formation is evidently the reaction that can provide the most important information on the spatial arrangement of atoms. Steric reasons should explain the observation that 5- or 6-membered chain undergoes ready closure, whereas a shorter or longer chain undergoes difficult or no closure.… The four valences of the carbon atom act in the directions that connect the center of a sphere with the corners of a tetrahedron and form angles of 109°28′ with one another. The direction of the attraction can deviate, but this in increasing strain as the sizes of the latter increase. ] This is the quintessence of the “ring-strain theory” formulated by Adolf von Baeyer over one hundred years ago. Although it is today only one facet of the many aspects of strain theory, it has repeatedly stimulated experimental and theoretical chemists. Among the most spectacular of the recent successes in synthetic chemistry are the syntheses of tetra-tert-butyltetrahedrane and [1.1.1]propellane. The reasons for the great stability of these two highly strained compounds are completely different. The experimental findings as well as the results of theoretical analysis by means of molecular mechanics and ab initio calculations have contributed decisively to our present state of knowledge of the structure, energy, and reactivity of organic compounds.}, + abstract = {Abstract “Die Ringschließung ist offenbar diejenige Erscheinung, welche am meisten über die räumliche Anordnung der Atome Auskunft geben kann. Wenn eine Kette von 5 und 6 Gliedern sich leicht, eine von weniger oder mehr Gliedern sich schwierig oder auch gar nicht schließen läßt, so müssen dafür offenbar räumliche Gründe vorhanden sein.… Die vier Valenzen des Kohlenstoffatoms wirken in den Richtungen, welche den Mittelpunkt der Kugel mit den Tetraederecken verbinden, und welche miteinander einen Winkel von 109°28′ machen. Die Richtung der Anziehung kann eine Ablenkung erfahren, die jedoch eine mit der Größe der Letzteren wachsende Spannung zur Folge hat,”[ Ring formation is evidently the reaction that can provide the most important information on the spatial arrangement of atoms. Steric reasons should explain the observation that 5- or 6-membered chain undergoes ready closure, whereas a shorter or longer chain undergoes difficult or no closure.… The four valences of the carbon atom act in the directions that connect the center of a sphere with the corners of a tetrahedron and form angles of 109 Degree 28′ with one another. The direction of the attraction can deviate, but this in increasing strain as the sizes of the latter increase. ] This is the quintessence of the “ring-strain theory” formulated by Adolf von Baeyer over one hundred years ago. Although it is today only one facet of the many aspects of strain theory, it has repeatedly stimulated experimental and theoretical chemists. Among the most spectacular of the recent successes in synthetic chemistry are the syntheses of tetra-tert-butyltetrahedrane and [1.1.1]propellane. The reasons for the great stability of these two highly strained compounds are completely different. The experimental findings as well as the results of theoretical analysis by means of molecular mechanics and ab initio calculations have contributed decisively to our present state of knowledge of the structure, energy, and reactivity of organic compounds.}, year = {1986} } @article{ilpmot, @@ -642,7 +640,7 @@ issn = {0098-1354}, doi = {https://doi.org/10.1016/j.compchemeng.2016.04.019}, url = {https://www.sciencedirect.com/science/article/pii/S0098135416301156}, - author = {Mark J. Willis and Moritz von Stosch}, + author = {Willis, Mark J. and von Stosch, Moritz }, keywords = {Chemical reaction network, Structural optimization, Kinetic fitting, Mixed-integer-linear programming}, abstract = {The manual determination of chemical reaction networks (CRN) and reaction rate equations is cumbersome and becomes workload prohibitive for large systems. In this paper, a framework is developed that allows an almost entirely automated recovery of sets of reactions comprising a CRN using experimental data. A global CRN structure is used describing all feasible chemical reactions between chemical species, i.e. a superstructure. Network search within this superstructure using mixed integer linear programming (MILP) is designed to promote sparse connectivity and can integrate known structural properties using linear constraints. The identification procedure is successfully demonstrated using simulated noisy data for linear CRNs comprising two to seven species (modelling networks that can comprise up to forty two reactions) and for batch operation of the nonlinear Van de Vusse reaction. A further case study using real experimental data from a biodiesel reaction is also provided.} } @@ -655,7 +653,7 @@ pages = {21590-21599}, year = {2025}, month = {12}, - abstract = { Human interpretation of spectroscopic data remains key to confirming newly synthesised chemical structures. Whilst there have been advances in automated spectral interpretation, the false positive and false negative rates remain too high to replace human interpretation. One approach, Automated Structure Verification (ASV), scores observed nuclear magnetic resonance (NMR) spectra against predicted NMR spectra. We describe a method to extend this approach to infrared (IR) spectra and apply it alongside proton NMR spectra to distinguish between a challenging set of 99 similar isomer pairs. Based on relative scores, we classify each as correct, incorrect or unsolved. Our results show that IR can be used as an efficient automated method to distinguish similar isomers with an accuracy close to that of proton NMR. We further introduce a method to combine NMR and IR results and show that the combination significantly outperforms either technique alone. At a true positive rate of 90\%, unsolved pairs are reduced to 0–15\% using NMR and IR together compared to 27–49\% using individual techniques alone. At a true positive rate of 95\%, they are reduced to 15–30\% from 39–70\%. These results are a significant step towards efficient automated structure verification based on easily measured spectroscopy data. }, + abstract = { Human interpretation of spectroscopic data remains key to confirming newly synthesised chemical structures. Whilst there have been advances in automated spectral interpretation, the false positive and false negative rates remain too high to replace human interpretation. One approach, Automated Structure Verification (ASV), scores observed nuclear magnetic resonance (NMR) spectra against predicted NMR spectra. We describe a method to extend this approach to infrared (IR) spectra and apply it alongside proton NMR spectra to distinguish between a challenging set of 99 similar isomer pairs. Based on relative scores, we classify each as correct, incorrect or unsolved. Our results show that IR can be used as an efficient automated method to distinguish similar isomers with an accuracy close to that of proton NMR. We further introduce a method to combine NMR and IR results and show that the combination significantly outperforms either technique alone. At a true positive rate of 90\%, unsolved pairs are reduced to 0–15\% using NMR and IR together compared to 27–49\% using individual techniques alone. At a true positive rate of 95 Percent, they are reduced to 15–30\% from 39–70\%. These results are a significant step towards efficient automated structure verification based on easily measured spectroscopy data. }, issn = {2041-6520}, doi = {10.1039/d5sc06866e}, url = {https://doi.org/10.1039/d5sc06866e},