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Customizing Axially-Oriented Dual-Atomic Synergy for Orchestrating Cascade Alkaline Hydrogen Evolution
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DOI：10.1002/adma.74458.png)
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Abstract
En 中文
The full orchestration of synergistic geometric and electronic interaction at atomic scale is fundamental to surmounting cascade kinetic bottlenecks inherent in multistep electrochemical processes. Here, an axially-oriented, sulfur-bridged hetero-atomic motif (Ru─S─Co) is customized to achieve synergistic regulation throughout alkaline hydrogen evolution reaction (HER). The top-positioned Ru atoms are tailored for enhanced water capture, and the bottom-inserted Co atoms in lattice activate middle S atoms for balanced hydrogen adsorption–desorption. This customized multi-site synergy conspicuously lowers the energy barrier for rate-determining water scission step. The proportion of reactive free water is elevated on this modified interface to prompt alkaline HER initiation. Furthermore, the intrinsically asymmetric charge distribution along the dual-atom bridge enhances charge transfer during HER, and the prominent orbital coupling induces an upshift in the Ru d-band center together with increased density of states in S p-orbitals around the Fermi level, further augmenting Ru-S dual-site activity. With this catalyst adopted as cathode, the anion-exchange-membrane electrolysis cell maintains an industrial current density of 1000 mA cm−2 at a small voltage of 1.79 V with negligible performance decay after long-term stability test. This work provides insights into precise customization of atomic-scale synergy toward effective management of kinetically mismatched multisteps in HER-related energy conversion.
Keywords:
atomic-site catalysts
electronic structure regulation
hydrogen evolution reaction
water electrolysis
Journal
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26.8
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3.4W
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46.0W