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Published on: December 6, 2021
Lewis-Acid-Rich ZrO2 as a High-Performance Support for Enabling Hydrogen Spillover for Enhanced Hydrogen Evolution
Qihao Wang1, Hongyue Diao1, Yusen Chen1
1Key Laboratory of Eco-Chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science & Technology, 53 Zhengzhou Road, Qingdao 266042, P. R. China.
None:
Hydrogen spillover offers a promising approach to develop highly active and affordable electrocatalysts for the hydrogen evolution reaction by regulating hydrogen migration and kinetics. Herein, a catalyst composed of osmium nanoparticles supported on zirconium dioxide (Os/ZrO2) is designed and synthesized. The Lewis-acid-rich ZrO2 support not only promotes water dissociation but also triggers hydrogen spillover, thereby optimizing the desorption energetics of hydrogen intermediates. Then, Os/ZrO2 delivers outstanding HER activity in both alkaline and acidic electrolytes, requiring overpotentials of only 16 and 14 mV to reach 10 mA cm-2, surpassing commercial Pt/C and Os/C. Mechanistic studies have confirmed the occurrence of hydrogen spillover, whereby hydrogen intermediates migrate from the Os nanoparticles to the ZrO2 surface, effectively tuning the adsorption/desorption kinetics and leading to significantly enhanced HER performance. Furthermore, in an anion-exchange membrane electrolyzer, Os/ZrO2||RuO2 achieves a low voltage of 1.82 V at 1 A cm-2 and maintains stable operation, translating to a hydrogen production cost of $0.97 per gasoline gallon equivalent. This work presents an effective strategy for designing high-performance HER catalysts through hydrogen spillover engineering, providing a feasible route for enhanced electrocatalytic systems.
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