Disentangling heterogeneous thermocatalytic formic acid dehydrogenation from an electrochemical perspective

Xianxian Qin, Jiejie Li, Tian-Wen Jiang, Xian-Yin Ma, Kun Jiang, Bo Yang (), Shengli Chen and Wen-Bin Cai ()
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Xianxian Qin: Fudan University
Jiejie Li: ShanghaiTech University
Tian-Wen Jiang: Fudan University
Xian-Yin Ma: Fudan University
Kun Jiang: Fudan University
Bo Yang: ShanghaiTech University
Shengli Chen: Wuhan University
Wen-Bin Cai: Fudan University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract Heterogeneous thermocatalysis of formic acid dehydrogenation by metals in solution is of great importance for chemical storage and production of hydrogen. Insightful understanding of the complicated formic acid dehydrogenation kinetics at the metal-solution interface is challenging and yet essential for the design of efficient heterogeneous formic acid dehydrogenation systems. In this work, formic acid dehydrogenation kinetics is initially studied from a perspective of electrochemistry by decoupling this reaction on Pd catalyst into two short-circuit half reactions, formic acid oxidation reaction and hydrogen evolution reaction and manipulating the electrical double layer impact from the solution side. The pH-dependences of formic acid dehydrogenation kinetics and the associated cation effect are attributed to the induced change of electric double layer structure and potential by means of electrochemical measurements involving kinetic isotope effect, in situ infrared spectroscopy as well as grand canonical quantum mechanics calculations. This work showcases how kinetic puzzles on some important heterogeneous catalytic reactions can be tackled by electrochemical theories and methodologies.

Date: 2024
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DOI: 10.1038/s41467-024-51926-1

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