Orbital engineering of C3N monolayer to design efficient synergistic sites electrocatalyst for boosting alkaline hydrogen evolution

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Zeng, Yamei
Zhang, Xu
Ai, Changzhi
Wang, Cai-Zhuang
Liu, Yipu
Lin, Shiwei
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Iowa State University Digital Repository, Ames IA (United States)
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

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Physics and Astronomy
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Alkaline water electrolyzer (AWE) is one of the promising technologies for hydrogen production at the industrial level. However, energetic inefficiency and low current density impede the development of AWE. Compared with acidic conditions, the Volmer step in alkaline hydrogen evolution reaction (HER) involves extra water dissociation, whose barrier is one of the most vital reasons for the sluggish kinetics of alkaline HER. Herein, choosing C3N monolayer as an ideal theoretical model, we design several empty orbitals through intentional metal doping, and further construct synergistic sites on the C3N monolayer to accelerate both water dissociation and hydrogen adsorption for alkaline HER. The as-designed Be-doped and Cr-doped C3N monolayers exhibit rather low theoretical overpotential of 0.476 eV and 0.216 eV for alkaline HER, respectively, which are even lower than Pt (1 1 1) surface. Moreover, by comparing the water dissociation behaviors on metal-doped C3N monolayer, we find that the empty orbitals with suitable orientation and energy level are useful for promoting the water dissociation process, indicating that we can use orbital engineering strategy to regulate the adsorption strength between adsorbate and surface site. Consequently, it is reasonable to suggest that our orbital engineering strategy would significantly benefit the design of highly efficient alkaline HER electrocatalysts.
This is a manuscript of an article published as Zeng, Yamei, Xu Zhang, Changzhi Ai, Caizhuang Wang, Yipu Liu, and Shiwei Lin. "Orbital engineering of C3N monolayer to design efficient synergistic sites electrocatalyst for boosting alkaline hydrogen evolution." Applied Surface Science 582 (2022): 152474. DOI: 10.1016/j.apsusc.2022.152474. Copyright 2022 Elsevier B.V. DOE Contract Number(s): AC02-07CH11358; 61764003; 22005116. Posted with permission.
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