Hydrogen evolution reaction on in-plane platinum and palladium dichalcogenides via single-atom doping. (20th May 2021)

• Record Type: Journal Article
• Authors: Liu, Gang; Li, Jingjing; Dong, Chao; Wu, Liyuan; Liang, Dan; Cao, Huawei; Lu, Pengfei
• Is Part Of: International journal of hydrogen energy. Volume 46:Number 35(2021)
• Page Start: 18294
• Page End: 18304
• Publication Date: 2021-05-20
• Subjects: Density functional theory -- Platinum and palladium dichalcogenides -- Single-atom doping -- Hydrogen evolution reaction; Hydrogen as fuel -- Periodicals; Hydrogène (Combustible) -- Périodiques; Hydrogen as fuel; Periodicals; 665.81
• DOI: 10.1016/j.ijhydene.2021.02.206
• Languages: English
• ISSNs: 0360-3199

Abstract

Abstract: Searching for the catalysts with excellent catalytic activity and high chemical stability is the key to achieve large-scale production of hydrogen (H2 ) through hydrogen evolution reaction (HER). Two-dimensional (2D) platinum and palladium dichalcogenides with extraordinary electrical properties have emerged as the potential candidate for HER catalysts. Here, chemical stability, HER electrocatalytic activity, and the origin of improved HER performance of Pt/Pd-based dichalcogenides with single-atom doping (B, C, N, P, Au, Ag, Cu, Co, Fe, Ni, Zn) and vacancies are explored by first-principles calculations. The calculated defect formation energy reveals that most defective structures are thermodynamically stable. Hydrogen evolution performance on basal plane is obviously improved by single-atoms doping and vacancies. Particularly, Zn-doped and Te vacancy PtTe2 have a Δ G H value close to zero. Moreover, defect engineering displays a different performance on HER catalytic activity in sulfur group elements, in order of S < Te < Se in Pd-based chalcogenides, and S < Se < Te in Pt-based chalcogenides. The origin of improved hydrogen evolution performance is revealed by electronic structure and charge transfer. Our findings of the highly activating defective systems provide a theoretical basis for HER applications of platinum and palladium dichalcogenides. Highlights: Pt/Pd-based dichalcogenides (MX2 ) with various atomic defects were constructed. The HER activity of MX2 basal plane is obviously improved by atomic defects. Zn-doped and Te vacancy PtTe2 show the optimal HER activity. Defect engineering displays a different performance in sulfur group elements.