P- or S-Doped graphdiyne as a superior metal-free electrocatalyst for the hydrogen evolution reaction: a computational study. (19th April 2021)

• Record Type: Journal Article
• Authors: Wang, Siyao; Jiao, Dongxu; Liu, Jingwei; Shang, Yongchen; Zhao, Jingxiang
• Is Part Of: New journal of chemistry. Volume 45:Number 18(2021)
• Page Start: 8101
• Page End: 8108
• Publication Date: 2021-04-19
• Subjects: Chemistry -- Periodicals; Chimie -- Périodiques; 540
• DOI: 10.1039/d1nj00652e
• Languages: English
• ISSNs: 1144-0546

Abstract

Abstract : By carefully controlling the type and site of the P or S dopant, graphdiyne can be utilized as a promising electrocatalyst with high efficiency for the hydrogen evolution reaction. Abstract : Searching for stable, efficient, and inexpensive metal-free electrocatalysts for the hydrogen evolution reaction (HER) is crucial for sustainable hydrogen generation. Herein, by means of density functional theory (DFT) computations, we proposed that P- or S-doping can effectively activate the basal plane of graphdiyne (GDY) for the HER. Our results revealed that these P- or S-doped GDY materials exhibit outstanding stability, enhanced electrical conductivity, and excellent magnetic properties. More interestingly, by carefully controlling the site and type of the P or S heteroatom, GDY can exhibit superior catalytic performance for the HER with the hydrogen adsorption free energy (Δ G H* ) being near zero, which can be attributed to its moderate p-band centers near the Fermi level. Our work highlights a novel metal-free electrocatalyst for the HER, providing a promising strategy to rationally design highly efficient HER catalysts for sustainable H2 production.