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An Overview of Glycerol Electrooxidation Mechanisms on Pt, Pd and Au
ChemSusChem ( IF 7.5 ) Pub Date : 2021-01-11 , DOI: 10.1002/cssc.202002669 Tianyu Li 1 , David A. Harrington 2
ChemSusChem ( IF 7.5 ) Pub Date : 2021-01-11 , DOI: 10.1002/cssc.202002669 Tianyu Li 1 , David A. Harrington 2
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In the most recent decade, glycerol electrooxidation (GEOR) has attracted extensive research interest for valorization of glycerol: the conversion of glycerol to value‐added products. These reactions at platinum, palladium, and gold electrodes have a lot of uncertainty in their reaction mechanisms, which has generated some controversies. This review gathers many reported experimental results, observations and proposed reaction mechanisms in order to draw a full picture of GEOR. A particular focus is the clarification of two propositions: Pd is inferior to Pt in cleaving the C−C bonds of glycerol during the electrooxidation and the massive production of CO2 at high overpotentials is due to the oxidation of the already‐oxidized carboxylate products. It is concluded that the inferior C−C bond cleavability with Pd electrodes, as compared with Pt electrodes, is due to the inefficiency of deprotonation, and the massive generation of CO2 as well as other C1/C2 side products is partially caused by the consumption of OH– at the anodes, as a lower pH reduces the amount of carboxylates and favors the C−C bond scission. A reaction mechanism is proposed in this review, in which the generation of side products are directly from glycerol (“competition” between each side product) rather than from the further oxidation of C2/C3 products. Additionally, GEOR results and associated interpretations for Ni electrodes are presented, as well as a brief review on the performances of multi‐metallic electrocatalysts (most of which are nanocatalysts) as an introduction to these future research hotpots.
中文翻译：
甘油在Pt，Pd和Au上的电氧化机理概述
在最近的十年中，甘油电氧化（GEOR）在甘油的增值方面引起了广泛的研究兴趣：将甘油转化为增值产品。在铂，钯和金电极上的这些反应在其反应机理上有很多不确定性，这引起了一些争议。这篇综述收集了许多报道的实验结果，观察结果和拟议的反应机理，以便全面了解GEOR。一个特别的重点是澄清两个命题：在电氧化和大量产生CO 2的过程中，Pd在裂解甘油的C-C键方面不如Pt。高电位的原因是已经氧化的羧酸盐产物被氧化。结论是，与Pt电极相比，Pd电极较差的C-C键裂解性是由于去质子效率低下所致，CO 2以及其他C1 / C2副产物的大量生成部分是由Pt电极引起的。 OH的消耗–在阳极处，由于较低的pH值会减少羧酸盐的含量并有利于C-C键断裂。在这篇综述中提出了一种反应机理，其中副产物的产生直接来自甘油（每种副产物之间的“竞争”），而不是C2 / C3产物的进一步氧化。此外，还介绍了GEOR结果和镍电极的相关解释，并简要介绍了多金属电催化剂（其中大多数是纳米催化剂）的性能，作为对这些未来研究热点的介绍。
更新日期：2021-01-11
中文翻译：
甘油在Pt，Pd和Au上的电氧化机理概述
在最近的十年中，甘油电氧化（GEOR）在甘油的增值方面引起了广泛的研究兴趣：将甘油转化为增值产品。在铂，钯和金电极上的这些反应在其反应机理上有很多不确定性，这引起了一些争议。这篇综述收集了许多报道的实验结果，观察结果和拟议的反应机理，以便全面了解GEOR。一个特别的重点是澄清两个命题：在电氧化和大量产生CO 2的过程中，Pd在裂解甘油的C-C键方面不如Pt。高电位的原因是已经氧化的羧酸盐产物被氧化。结论是，与Pt电极相比，Pd电极较差的C-C键裂解性是由于去质子效率低下所致，CO 2以及其他C1 / C2副产物的大量生成部分是由Pt电极引起的。 OH的消耗–在阳极处，由于较低的pH值会减少羧酸盐的含量并有利于C-C键断裂。在这篇综述中提出了一种反应机理，其中副产物的产生直接来自甘油（每种副产物之间的“竞争”），而不是C2 / C3产物的进一步氧化。此外，还介绍了GEOR结果和镍电极的相关解释，并简要介绍了多金属电催化剂（其中大多数是纳米催化剂）的性能，作为对这些未来研究热点的介绍。
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