中国物理B ›› 2023, Vol. 32 ›› Issue (6): 66106-066106.doi: 10.1088/1674-1056/aca7ec

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Hydrogen evolution reaction between small-sized Zrn (n = 2–5) clusters and water based on density functional theory

Lei-Lei Tang(唐雷雷)1, Shun-Ping Shi(史顺平)1,†, Yong Song(宋永)1,‡, Jia-Bao Hu(胡家宝)1, Kai Diao(刁凯)1, Jing Jiang(蒋静)1, Zhan-Jiang Duan(段湛江)1, and De-Liang Chen(陈德良)2   

  1. 1 College of Mathematics and Physics, Chengdu University of Technology, Chengdu 610059, China;
    2 School of Physics and Electronics, Guizhou Education University, Guiyang 550018, China
  • 收稿日期:2022-09-26 修回日期:2022-11-14 接受日期:2022-12-02 出版日期:2023-05-17 发布日期:2023-06-07
  • 通讯作者: Shun-Ping Shi, Yong Song E-mail:shishunping13@cdut.edu.cn;syong@cdut.edu.cn
  • 基金资助:
    Project supported by the Open Research Fund of Computational Physics Key Laboratory of Sichuan Province, Yibin University, China (Grant No. YBXYJSWL-ZD-2020-005) and the Student’s Platform for Innovation and Entrepreneurship Training Program, China (Grant No. S202110616084).

Hydrogen evolution reaction between small-sized Zrn (n = 2–5) clusters and water based on density functional theory

Lei-Lei Tang(唐雷雷)1, Shun-Ping Shi(史顺平)1,†, Yong Song(宋永)1,‡, Jia-Bao Hu(胡家宝)1, Kai Diao(刁凯)1, Jing Jiang(蒋静)1, Zhan-Jiang Duan(段湛江)1, and De-Liang Chen(陈德良)2   

  1. 1 College of Mathematics and Physics, Chengdu University of Technology, Chengdu 610059, China;
    2 School of Physics and Electronics, Guizhou Education University, Guiyang 550018, China
  • Received:2022-09-26 Revised:2022-11-14 Accepted:2022-12-02 Online:2023-05-17 Published:2023-06-07
  • Contact: Shun-Ping Shi, Yong Song E-mail:shishunping13@cdut.edu.cn;syong@cdut.edu.cn
  • Supported by:
    Project supported by the Open Research Fund of Computational Physics Key Laboratory of Sichuan Province, Yibin University, China (Grant No. YBXYJSWL-ZD-2020-005) and the Student’s Platform for Innovation and Entrepreneurship Training Program, China (Grant No. S202110616084).

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摘要： Density functional theory (DFT) is used to calculate the most stable structures of Zr$_{n }$ ($n=2$-5) clusters as well as the adsorption energy values of Zr$_{n }$ ($n=2$-5) clusters after adsorbing single water molecule. The results reveal that there is a significant linear relationship between the adsorption energy values and the energy gaps of the Zr$_{n }$ ($n=2$-5) clusters. Furthermore, the calculations of the reaction paths between Zr$_{n}$ ($n=2$-5) and single water molecule show that water molecule can react with Zr$_{n}$ ($n=2$-5) clusters to dissociate, producing hydrogen, and O atoms mix with the clusters to generate Zr$_{n}$O ($n=2$-5), all of which are exothermic reactions. According to the released energy, the Zr$_{4}$ cluster is the most efficient in Zr$_{n}$ ($n=2$-5) clusters reacting with single water molecule. The natural population analysis (NPA) and density of states (DOS) demonstrate the production of hydrogen and orbital properties in different energy ranges, respectively, jointly forecasting that Zr$_{n}$O ($n= 2$-5) will probably continue to react with more water molecules. Our findings contribute to better understanding of Zr's chemical reactivity, which can conduce to the development of effective Zr-based catalysts and hydrogen-production methods.

关键词: density functional theory, hydrogen evolution reaction, NBO analysis, reaction pathways

Abstract: Density functional theory (DFT) is used to calculate the most stable structures of Zr$_{n }$ ($n=2$-5) clusters as well as the adsorption energy values of Zr$_{n }$ ($n=2$-5) clusters after adsorbing single water molecule. The results reveal that there is a significant linear relationship between the adsorption energy values and the energy gaps of the Zr$_{n }$ ($n=2$-5) clusters. Furthermore, the calculations of the reaction paths between Zr$_{n}$ ($n=2$-5) and single water molecule show that water molecule can react with Zr$_{n}$ ($n=2$-5) clusters to dissociate, producing hydrogen, and O atoms mix with the clusters to generate Zr$_{n}$O ($n=2$-5), all of which are exothermic reactions. According to the released energy, the Zr$_{4}$ cluster is the most efficient in Zr$_{n}$ ($n=2$-5) clusters reacting with single water molecule. The natural population analysis (NPA) and density of states (DOS) demonstrate the production of hydrogen and orbital properties in different energy ranges, respectively, jointly forecasting that Zr$_{n}$O ($n= 2$-5) will probably continue to react with more water molecules. Our findings contribute to better understanding of Zr's chemical reactivity, which can conduce to the development of effective Zr-based catalysts and hydrogen-production methods.

Key words: density functional theory, hydrogen evolution reaction, NBO analysis, reaction pathways

中图分类号:  (Structure of clusters (e.g., metcars; not fragments of crystals; free or loosely aggregated or loosely attached to a substrate))

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