Engineering a local acid-like environment in alkaline medium for efficient hydrogen evolution reaction

Hao Tan, Bing Tang, Ying Lu, Qianqian Ji, Liyang Lv, Hengli Duan, Na Li, Yao Wang, Sihua Feng, Zhi Li, Chao Wang (), Fengchun Hu, Zhihu Sun () and Wensheng Yan ()
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Hao Tan: University of Science and Technology of China
Bing Tang: University of Science and Technology of China
Ying Lu: University of Science and Technology of China
Qianqian Ji: University of Science and Technology of China
Liyang Lv: University of Science and Technology of China
Hengli Duan: University of Science and Technology of China
Na Li: University of Science and Technology of China
Yao Wang: University of Science and Technology of China
Sihua Feng: University of Science and Technology of China
Zhi Li: University of Science and Technology of China
Chao Wang: University of Science and Technology of China
Fengchun Hu: University of Science and Technology of China
Zhihu Sun: University of Science and Technology of China
Wensheng Yan: University of Science and Technology of China

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Tuning the local reaction environment is an important and challenging issue for determining electrochemical performances. Herein, we propose a strategy of intentionally engineering the local reaction environment to yield highly active catalysts. Taking Ptδ− nanoparticles supported on oxygen vacancy enriched MgO nanosheets as a prototypical example, we have successfully created a local acid-like environment in the alkaline medium and achieve excellent hydrogen evolution reaction performances. The local acid-like environment is evidenced by operando Raman, synchrotron radiation infrared and X-ray absorption spectroscopy that observes a key H3O+ intermediate emergence on the surface of MgO and accumulation around Ptδ− sites during electrocatalysis. Further analysis confirms that the critical factors of the forming the local acid-like environment include: the oxygen vacancy enriched MgO facilitates H2O dissociation to generate H3O+ species; the F centers of MgO transfers its unpaired electrons to Pt, leading to the formation of electron-enriched Ptδ− species; positively charged H3O+ migrates to negatively charged Ptδ− and accumulates around Ptδ− nanoparticles due to the electrostatic attraction, thus creating a local acidic environment in the alkaline medium.

Date: 2022
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DOI: 10.1038/s41467-022-29710-w

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