Sulfur-mediated transformation from osmium nanocrystals to single atoms for efficient alkaline hydrogen evolution reaction
Abstract
Osmium (Os)-based catalysts, recognized for their unique chemical and electronic properties along with cost-effectiveness, hold great potential for the hydrogen evolution reaction (HER). However, their practical application has long been limited because pure Os exhibits excessively strong adsorption of intermediates and suffers from stability issues. Herein, we report the development of a highly stable catalyst achieved by implanting the sulfur (S) atom into the matrix, facilitating the transformation of Os nanocrystals into Os single atoms. The prepared atomically dispersed Os catalyst (Os-SA@SNC) demonstrates outstanding catalytic activity, requiring only a 13 mV overpotential to achieve a current density of 10 mA cm −2 in 1.0 M potassium hydroxide (KOH) solution, as well as the excellent durability. This performance surpasses that of commercial Pt/C and outperforms most of the reported state-of-the-art electrocatalysts. Theoretical simulations clarify the important role of S atoms in promoting the dispersion and diffusion of Os atoms. Moreover, density functional theory calculations indicate that S atoms adjust the local electronic structure of Os active sites, further facilitating the adsorption/dissociation of H 2 O and optimizing the hydrogen adsorption free energy (ΔG *H ), thereby accelerating the kinetics of both the Volmer and Heyrovsky steps in alkaline HER. This work revitalizes Os-based catalysts for energy conversion and paves the way for innovative HER catalyst design and application to contaminated soil/water remediation.
Article Details
Journal Info
Proceedings of the National Academy of Sciences
National Academy of Sciences
Authors (15)
Wendan Xue
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Qixing Zhou
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Pengfei Wang
Key Laboratory of Photochemical Conversion and Optoelectronic Materials
Sijin Zuo
State of Key Laboratory of Natural Medicines School of Engineering, China Pharmaceutical University
Fengxiang Li
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Jiwei Jiang
North China Municipal Engineering Design and Research Institute Co. Ltd. Beijing Branch
Fan Mo
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Chuan Yin
Gaolei Liu
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Zhan Ban
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Yuanyuan Wei
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Wen An
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Xiulin Huang
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University
Hui Wang
Sihui Zhan
Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Carbon Neutrality Interdisciplinary Science Centre/College of Environmental Science and Engineering, Nankai University