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An Overview of Glycerol Electrooxidation Mechanisms on Pt, Pd and Au

CHEMSUSCHEM (2021)

Journal

CHEMSUSCHEM

Volume 14, Issue 6, Pages 1472-1495

Publisher

WILEY-V C H VERLAG GMBH

DOI: 10.1002/cssc.202002669

Keywords

carboxylic acids; glycerol oxidation; gold; palladium; platinum

Funding

Natural Sciences and Engineering Research Council of Canada through its Discovery Frontiers program (Engineered Nickel Catalysts for Electrochemical Clean Energy project (Ni Electro Can))
Natural Sciences and Engineering Research Council of Canada through CREATE program (Materials for Enhanced Energy Technologies (MEET) project)
Research Council of Norway through its International Partnerships Program (Canada-Norway Partnership in Electrochemical Energy Technologies (CANOPENER) project)
Natural Sciences and Engineering Research Council of Canada

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Abstract

This review discusses the reaction mechanisms of glycerol electrooxidation, emphasizing the inferiority of Pd compared to Pt electrodes in cleaving glycerol C-C bonds and the reasons for CO2 generation at high overpotentials. A new reaction mechanism is proposed to explain the generation of side products. Additionally, experimental results for Ni electrodes and the performance of multi-metallic electrocatalysts are presented.

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.

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