Mutual-Activation between Doped Pt-Single-Atoms and Basal-Plane Sites in 1T-TaS2 Nanosheets Networks for Highly Efficient Hydrogen Evolution

作者：Peng You, Xinying Yang, Yahuan Huan, Jialong Wang, Tong Zhou, Haiping Lin, Jianyu Cao, Haoxuan Ding, Jiatian Fu, Yujin Cheng, Xing Fan, Jing Xia, Yanfeng Zhang · 发表于：ACS Nano · 年份：2025 · DOI：10.1021/acsnano.5c11863 · 被引用次数：4 · 研究领域：Molecular Junctions and Nanostructures、Advanced Chemical Physics Studies、Machine Learning in Materials Science

Doping single atoms (SAs) into catalytically active substrates offers the possibility for both SAs and substrates to co-participate in the catalytic reactions (e.g., hydrogen evolution (HER)) toward highly improved overall performance. Semiconducting transition-metal dichalcogenides (TMDCs), especially MoS 2, have been selected as active substrates; however, their restricted edge-active sites and insufficient electronic modulation of SAs limit their practical applications. Herein, we report the preparation of Pt-SAs doped 1T-TaS 2 nanosheets catalysts via chemical vapor deposition followed by electrochemical deposition. The vertically aligned 1T-TaS 2 nanosheet networks can afford abundant edge and basal-plane active sites, and the low electronegativity of Ta enables effective modulation of the electronic structure of doped Pt-SAs. Notably, the designed catalyst exhibits comparable overpotential (∼145 mV at 100 mA cm –2 ) and Tafel slope (∼33.8 mV dec –1 ) to commercial Pt/C, while demonstrating 40-times higher Pt mass activity (∼10.92 A mg –1 at 50 mV). Further density functional theory calculations reveal a mutual-activation mechanism; i.e., the Pt-SAs activate the basal-plane sites of TaS 2 and vice versa, inducing a synergistic enhancement of the HER performance. This work hereby discusses the fundamental mechanisms of Pt-SAs and TMDCs co-catalytic systems and offers design principles of high-efficiency and cost-effective HER catalysts.