Alternative Reaction Channels and Carbene Intermediates in the Ce~(4+) - Malonic Acid and Ce~(4_) - Bromomalonic Acid Reactions. 1. CO_2 Measurements

Szilveszter Nagygyory; Maria Wittmann; Szilveszter Pinter; Andras Visegrady; Andras Dancso; Nguyen Bich Thuy; Zoltan Noszticzius; Laszlo Hegedus; Horst-Dieter Forsterling

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Alternative Reaction Channels and Carbene Intermediates in the Ce~(4+) - Malonic Acid and Ce~(4_) - Bromomalonic Acid Reactions. 1. CO_2 Measurements

机译：Ce〜（4 +）-丙二酸和Ce〜（4 _）-溴丙二酸反应中的替代反应通道和卡宾中间体。 1. CO_2测量

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The Ce~(4+)-malonic/bromomalonic acid reactions play an important role in the oscillatory Belousov-Zhabotinsky reaction. In this work CO_2 evolution from these reactions was studied with a sensitive and quantitative method, by converting the CO_2 to methane and measuring it with a flame ionization detector. It was found that the stoichiometries depend on the initial conditions in batch experiments or on the mixing rate of reagents in a semibatch reactor. These findings are explained by two main reaction channels: one for recombination and another for decarboxylation. Decarboxylation itself has two separate routes, one is dominant at low while the other at high Ce~(4+) concentrations. In the latter, formation of more than two CO_2 molecules from one malonic/bromomalonic acid molecule was observed. Novel reaction schemes containing carbenes are proposed for these "high Ce~(4+) " decarboxylation channels. To check the new mechanism, HPLC measurements are planned as a continuation of the research.

机译：Ce〜（4 +）-丙二酸/溴丙二酸反应在振荡的Belousov-Zhabotinsky反应中起重要作用。在这项工作中，通过灵敏和定量的方法研究了从这些反应中释放出的CO_2，方法是将CO_2转化为甲烷，并使用火焰离子化检测器进行测量。发现化学计量学取决于间歇实验中的初始条件或取决于半间歇反应器中试剂的混合速率。这些发现由两个主要的反应通道解释：一个用于重组，另一个用于脱羧。脱羧作用本身有两种不同的途径，一种途径在低浓度下占优势，另一种途径在高Ce〜（4+）浓度下。在后者中，观察到由一个丙二酸/溴丙二酸分子形成两个以上的CO_2分子。针对这些“高Ce〜（4+）”脱羧通道，提出了含有碳烯的新型反应方案。为了检查新机制，计划将HPLC测量作为研究的延续。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |1999年第25期|共8页
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Szilveszter Nagygyory; Maria Wittmann; Szilveszter Pinter; Andras Visegrady; Andras Dancso; Nguyen Bich Thuy; Zoltan Noszticzius; Laszlo Hegedus; Horst-Dieter Forsterling;
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中图分类物理化学（理论化学）、化学物理学;
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1. Alternative Reaction Channels and Carbene Intermediates in the Ce~(4+) - Malonic Acid and Ce~(4_) - Bromomalonic Acid Reactions. 1. CO_2 Measurements [J] . Szilveszter Nagygyory, Maria Wittmann, Szilveszter Pinter, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 1999,第25期

机译：Ce〜（4 +）-丙二酸和Ce〜（4 _）-溴丙二酸反应中的替代反应通道和卡宾中间体。 1. CO_2测量
2. Contribution to the chemistry of the Belousov-Zhabotinsky reaction products of the ferriin-bromomalonic acid and the ferriin-malonic acid reactions [J] . Hegedus L, Forsterling HD, Onel L, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2006,第47期

机译：铁蛋白-溴丙二酸和铁蛋白-丙二酸反应的Belousov-Zhabotinsky反应产物的化学贡献
3. Contribution to the chemistry of the Belousov-Zhabotinsky reaction products of the ferriin-bromomalonic acid and the ferriin-malonic acid reactions [J] . Hegedus L, Forsterling HD, Onel L, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2006,第47期

机译：铁蛋白-溴丙二酸和铁蛋白-丙二酸反应的Belousov-Zhabotinsky反应产物的化学贡献
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Alternative Reaction Channels and Carbene Intermediates in the Ce~(4+) - Malonic Acid and Ce~(4_) - Bromomalonic Acid Reactions. 1. CO_2 Measurements

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