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; Mengning Ding

doi:10.1038/s41467-022-34685-9

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

Nat Commun. 2022 Nov 14;13(1):6911. doi: 10.1038/s41467-022-34685-9.

Authors

Zhangyan Mu^#¹, Na Han^#^{2

3}, Dan Xu⁴, Bailin Tian¹, Fangyuan Wang¹, Yiqi Wang¹, Yamei Sun¹, Cheng Liu¹, Panke Zhang⁵, Xuejun Wu⁴, Yanguang Li^{6

7}, Mengning Ding⁸

Affiliations

¹ Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, P. R. China.
² Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, P. R. China.
³ Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Suzhou, China.
⁴ State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, P. R. China.
⁵ State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, P. R. China.
⁶ Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, P. R. China. [email protected].
⁷ Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Suzhou, China. [email protected].
⁸ Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, P. R. China. [email protected].

^# Contributed equally.

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 pK_a) on the hydrogen sorption kinetics during CO₂RR, which offer additional insights into the electrochemical interfaces and optimization of the catalytic systems.

Abstract

Grants and funding