Critical role of hydrogen sorption kinetics in electrocatalytic CO2 reduction revealed by on-chip in situ transport investigations

Zhangyan Mu, Na Han, Dan Xu, Bailin Tian, Fangyuan Wang, Yiqi Wang, Yamei Sun, Cheng Liu, Panke Zhang, Xuejun Wu, Yanguang Li () and Mengning Ding ()
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Zhangyan Mu: Nanjing University
Na Han: Soochow University
Dan Xu: Nanjing University
Bailin Tian: Nanjing University
Fangyuan Wang: Nanjing University
Yiqi Wang: Nanjing University
Yamei Sun: Nanjing University
Cheng Liu: Nanjing University
Panke Zhang: Nanjing University
Xuejun Wu: Nanjing University
Yanguang Li: Soochow University
Mengning Ding: Nanjing University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Precise understanding of interfacial metal−hydrogen interactions, especially under in operando conditions, is crucial to advancing the application of metal catalysts in clean energy technologies. To this end, while Pd-based catalysts are widely utilized for electrochemical hydrogen production and hydrogenation, the interaction of Pd with hydrogen during active electrochemical processes is complex, distinct from most other metals, and yet to be clarified. In this report, the hydrogen surface adsorption and sub-surface absorption (phase transition) features of Pd and its alloy nanocatalysts are identified and quantified under operando electrocatalytic conditions via on-chip electrical transport measurements, and the competitive relationship between electrochemical carbon dioxide reduction (CO2RR) and hydrogen sorption kinetics is investigated. Systematic dynamic and steady-state evaluations reveal the key impacts of local electrolyte environment (such as proton donors with different pKa) on the hydrogen sorption kinetics during CO2RR, which offer additional insights into the electrochemical interfaces and optimization of the catalytic systems.

Date: 2022
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DOI: 10.1038/s41467-022-34685-9

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