Xuan-Yi Zhu, Shui-Zhong Zhao, Xue-Feng Zhang, Xia Huang, Cheng-Juan Gao, Li-Hong Yu, Zi-Yi Du, Li-Ming Cao, Chun-Ting He
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引用次数: 0
Abstract
Transition metal phosphides (TMPs) are high-potential catalysts for hydrogen evolution reaction (HER) yet struggle with the long-term maintenance of high activity at ampere-level current densities. Size cutting and heteroatom modification of TMPs are effective ways to improve their surface affinities and catalytic efficiencies, but the particle stabilities and synergistic regulation of band structures at different sites have become huge challenges. Herein, we have successfully synthesized cluster-level sulfur-doped iridium diphosphide (S-IrP2) through a molecular engineering strategy. It requires only low overpotentials of 133.6 ± 1.2 and 217.2 ± 2.6 mV to drive industrial current densities of 1.0 and 2.0 A·cm–2, respectively, being one of the best alkaline HER catalyst. Moreover, it showed almost no activity loss over 20,000 cycles and exhibited a remarkable charge transfer amount that exceeds those of reported TMPs. The electronic tailoring of IrP2 by sulfur atoms enables simultaneous shifting of the d-band and f-band centers of Ir and the p-band center of P, which co-optimizes the H and OH adsorption to lowering the H migration and H2 formation barriers. This work demonstrates that the molecular confinement synthesis holds tremendous prospects for architecting ultrafine metallic compounds with re-definable active surfaces.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.