Contribution to the chemistry of the Belousov-Zhabotinsky reaction products of the ferriin-bromomalonic acid and the ferriin-malonic acid reactions

Hegedus L; Forsterling HD; Onel L; Wittmann M; Noszticzius Z

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Contribution to the chemistry of the Belousov-Zhabotinsky reaction products of the ferriin-bromomalonic acid and the ferriin-malonic acid reactions

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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In the present mechanistic schemes of the ferroin-catalyzed oscillatory Belousov-Zhabotinsky (BZ) reaction the oxidation of the organic substrates (bromomalonic or malonic acid) by ferriin (the oxidized form of the catalyst) plays an important role. As the organic products of these reactions were not yet identified experimentally, they were studied here by an HPLC technique. It was found that the main organic oxidation product of bromomalonic acid is bromo-ethene-tricarboxylic acid (BrEETRA), the same compound that is formed when bromomalonic acid is oxidized by Ce4+ (another catalyst of the BZ reaction). Formation of BrEETRA is explained here by a new mechanism that is more realistic than the one suggested earlier. To find any oxidation product of malonic acid in the ferriin-malonic acid reaction was not successful, however. Neither ethane-tetracarboxylic acid (ETA) nor malonyl malonate (MAMA), the usual products of the Ce4+ -malonic acid reaction, nor any other organic acid, not even CO2, was found as a product of the reaction. We propose that malonic acid is not oxidized in the ferriin-malonic acid reaction, and it plays only the role of a complex forming catalyst in a process where Fe3+ oxidizes mostly its phenantroline ligand.

机译：在铁蛋白催化的振荡Belousov-Zhabotinsky（BZ）反应的当前机理方案中，铁蛋白（催化剂的氧化形式）对有机底物（溴代丙二酸或丙二酸）的氧化起着重要的作用。由于尚未通过实验鉴定这些反应的有机产物，因此在这里通过HPLC技术对其进行了研究。发现溴代丙二酸的主要有机氧化产物是溴代乙烯-三羧酸（BrEETRA），与溴代丙二酸被Ce4 +（BZ反应的另一种催化剂）氧化时形成的化合物相同。 BrEETRA的形成在这里通过一种新的机制进行了解释，该机制比先前提出的机制更为现实。然而，在铁蛋白-丙二酸反应中发现丙二酸的任何氧化产物是不成功的。 Ce4 +-丙二酸反应的常用产物乙烷-四羧酸（ETA）或丙二酸丙二酸酯（MAMA）均未发现该反应的产物，甚至没有任何其他有机酸，甚至是CO2。我们提出丙二酸在铁蛋白-丙二酸反应中不被氧化，并且在Fe3 +主要氧化其菲咯啉配体的过程中仅起络合物形成催化剂的作用。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2006年第47期|共6页
作者
Hegedus L; Forsterling HD; Onel L; Wittmann M; Noszticzius Z;
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正文语种 eng
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OSCILLATORY BZ REACTION; CE4+-MALONIC ACID; ORGANIC SUBSET; REACTION CHANNELS; CHEMICAL SYSTEMS; HPLC; OXIDATION; REDUCTION; BROMATE; CERIUM;

机译：振荡BZ反应;CE4 +-苹果酸;有机亚基;反应通道;化学体系;HPLC;氧化;还原;溴酸盐;铈;

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1. 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
2. Uncatalyzed Reactions in the Classical Belousov-Zhabotinsky System.I.Reactions of Bromomalonic Acid with Acidic Bromate and with HOBr [J] . Lavinia Onel, Gelu Bourceanu, Maria Wittmann, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2005,第45期

机译：Belousov-Zhabotinsky经典体系中的未催化反应.I。溴代丙二酸与酸性溴酸盐和HOBr的反应
3. Uncatalyzed Reactions in the Classical Belousov-Zhabotinsky System.2.The Malonic Acid-Bromate Reaction in Acidic Media [J] . Lavinia Onel, Gelu Bourceanu, Istvan Bitter, The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory . 2006,第3期

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Contribution to the chemistry of the Belousov-Zhabotinsky reaction products of the ferriin-bromomalonic acid and the ferriin-malonic acid reactions

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