文献类型：期刊文献

英文题名：Atomic-distancing control via layer-dislocation engineering breaks OER/ ORR activity limits in bilayer single-atom catalysts

作者：Lu, Xinyi[1,2];Huang, Haicai[1,3];Bao, Yihui[2];Xia, Yanyan[2];Chen, Xi[1,3];Ye, Zhencheng[2];Chen, Houyang[1,3]

机构：[1]Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]Univ Chinese Acad Sci, Chongqing Sch, Chongqing 400714, Peoples R China

年份：2026

卷号：715

外文期刊名：APPLIED SURFACE SCIENCE

收录：;EI(收录号：20253819192390);WOS:【SCI-EXPANDED(收录号:WOS:001575486500005)】；

基金：This work is supported by Geological Disaster Patterns and Mitigation Strategies Under River-Reservoir Hydrodynamics in the Three Gorges Reservoir Fluctuation Zone (5000002024CC20004), Natural Science Foundation of Chongqing (CSTB2023NSCQ-MSX0045), Postdoctoral Program of Natural Science Foundation of Chongqing (CSTB2023NSCQ-BHX0231), the Startup Foundation of Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences. The authors acknowledge hzwtech (www.hzwtech.com) for providing HPC resources that have contributed to the research results reported within this paper.

语种：英文

外文关键词：Bilayer single-atom catalysts; Linear scaling relationships; Oxygen reduction reaction; Oxygen evolution reaction; Layer-dislocation

摘要：Despite intensive efforts, electrocatalyst design remains constrained by the persistent activity-stability trade-off and the limitations imposed by linear scaling relationships (LSR) governing oxygen evolution/reduction reactions (OER/ORR). To overcome these challenges, we demonstrate a layer-dislocation strategy for bilayer single-atom catalysts (BSACs) that enables atomic-scale control of metal-metal spacing (dM-M) via interlayer dislocation modulation (Delta x). This geometric engineering directly regulates charge transfer and optimizes activesite electronic structures, breaking LSR to achieve low overpotentials. Crucially, we reveal metal-categorydependent mechanisms: -in strongly correlated systems (Mn/Fe/Co and their congeners), dislocation shifts dorbital energy level toward the Fermi level, strengthening intermediate adsorption; in weakly correlated systems (Ni/Cu and their congeners), van der Waals-driven structural perturbation disrupts LSR constraints. This work provides a metal-specific design framework for next-generation electrocatalysts by harnessing dislocationinduced electronic tailoring.