Electrocatalytic hydrogen evolution performance of modified Ti3C2O2 doped with non-metal elements: A DFT study
Zhongxiao Wang,
Haoxiang Di,
Rui Sun,
Yuting Zhu,
Longwei Yin,
Zhiwei Zhang,
Chengxiang Wang
Affiliations
Zhongxiao Wang
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Haoxiang Di
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Rui Sun
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Yuting Zhu
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Longwei Yin
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Zhiwei Zhang
Corresponding Authors.; Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Chengxiang Wang
Corresponding Authors.; Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
Developing highly conductive, stable, and active hydrogen evolution reaction (HER) catalysts is a critical step towards establishing the hydrogen economy. However, there are few catalysts, except for noble metals, that can meet all the requirements. Recently, two-dimensional (2D) transition metal carbon/nitride (MXene) materials have shown excellent performance in catalysis, and have attracted wide attention from researchers. In this study, the effectiveness of non-metal element (B, C, N, P, and S)-doped Ti3C2O2 MXene in the electrocatalytic hydrogen evolution reaction was investigated using density functional theory (DFT) calculations. Non-metal atoms as electron donors can provide additional electrons to the O functional group on the catalyst surface, thereby reducing charge transfer from H to O and the interaction between H and O. The Gibbs free energy (∆GH) of non-metal element-doped Ti3C2O2 is closer to 0 than that of pristine Ti3C2O2, demonstrating better hydrogen evolution performance. Furthermore, in the hydrogen evolution path, the desorption process is more inclined to the Heyrovsky mechanism, and doping greatly reduces the energy barrier of the reaction, thereby improving the catalytic efficiency. The present results prove that doping with non-metallic elements is an effective means of improving the catalytic activity of Ti3C2O2 for hydrogen evolution.
