Surface Van Hove Singularity Enabled Efficient Catalysis in Low-Dimensional Systems: CO Oxidation and Hydrogen Evolution Reactions

Liangliang Liu; Chunyan Wang; Liying Zhang; Chengyan Liu; Chunyao Niu; Zaiping Zeng; Dongwei Ma; Yu Jia

doi:10.1021/acs.jpclett.1c03861

Surface Van Hove Singularity Enabled Efficient Catalysis in Low-Dimensional Systems: CO Oxidation and Hydrogen Evolution Reactions

J Phys Chem Lett. 2022 Jan 27;13(3):740-746. doi: 10.1021/acs.jpclett.1c03861. Epub 2022 Jan 14.

Authors

Liangliang Liu^{1

2}, Chunyan Wang^{1

3}, Liying Zhang¹, Chengyan Liu¹, Chunyao Niu³, Zaiping Zeng¹, Dongwei Ma^{1

2}, Yu Jia^{1

3

2}

Affiliations

¹ Key Laboratory for Special Functional Materials of Ministry of Education, Collaborative Innovation Center of Nano Functional Materials and Applications, School of Materials, Henan University, Kaifeng 475004, China.
² Key Laboratory for Quantum Materials of Henan, and Center for Topological Functional Materials, Henan University, Kaifeng 475004, China.
³ International Laboratory for Quantum Functional Materials of Henan, and School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450001, China.

PMID: 35029120
DOI: 10.1021/acs.jpclett.1c03861

Abstract

Surface Van Hove singularity (SVHS) triggers exciting physical phenomena distinct from the bulk. Herein, we explore the potential role of SVHS in catalysis for both CO oxidation and the hydrogen evolution reaction (HER) using the graphene/Ca₂N (Gra/Ca₂N) heterojunction and Pt₂HgSe₃ (001) surface as prototype systems. It is demonstrated that both systems with SVHS could serve as an electron bath to promote O₂ adsorption and subsequent CO oxidation with low energy barriers of 0.2-0.6 eV for the Gra/Ca₂N and Pt₂HgSe₃ (001) surface and similarly facilitate the HER with near-zero hydrogen adsorption free energy. Importantly, the catalytically active sites associated with SVHS are well-defined and distributed over the whole surface plane, and further, the chemical reactivity of SVHS can also be tuned easily via adjusting its position with respect to E_F. Our study demonstrates the enabling power of SVHS and provides novel physical insights into the promising potential role of VHS in designing high-efficiency catalysts.