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

Title：

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

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^2,3* &   Mengning Ding¹*

Institutions：

¹Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

²Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, P. R. China.

³Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Suzhou, China.

⁴State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

⁵State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

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.

IF：

14.919

Link：

https://doi.org/10.1038/s41467-022-34685-9