文献类型：期刊文献

英文题名：Synergistic space-electron regulation under interlayer confinement: Disrupting oxygen evolution/reduction reaction scaling relations via dual-pathway control

作者：Lu, Xinyi[1,2];Huang, Haicai[1,3];Bao, Yihui[2];Xia, Yanyan[2];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 Informat Sci & Engn, Shanghai 200237, Peoples R China;[3]Univ Chinese Acad Sci, Chongqing Sch, Chongqing 400714, Peoples R China

年份：2026

卷号：710

外文期刊名：JOURNAL OF COLLOID AND INTERFACE SCIENCE

收录：;EI(收录号：20260620042180);WOS:【SCI-EXPANDED(收录号:WOS:001685643400001)】；

基金：This work is supported by Geological Disaster Patterns and Mitiga tion Strategies Under River-Reservoir Hydrodynamics in the Three Gorges Reservoir Fluctuation Zone (5000002024CC20004) , Natural Science Foundation of Chongqing (CSTB2023NSCQ-MSX0045) , the Startup Foundation of Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences. Computations were per-formed on Hefei advanced computing center. The authors acknowledge Beijing PARATERA Tech CO., Ltd. for providing HPC resources that have contributed to the research results reported within this paper.

语种：英文

外文关键词：Linear scaling relationship; Interlayer confinement engineering; Oxygen evolution reaction; Oxygen reduction reaction

摘要：Oxygen evolution and reduction reactions (OER/ORR) are fundamental to energy conversion technologies such as water electrolyzers and fuel cells. However, the intrinsic linear scaling relationship (LSR) between the intermediate adsorption energies limits catalytic activity. Overcoming this limitation could surpass the conventional activity-volcano relationship and unlock high-performance OER/ORR electrocatalysts. Herein, we propose a novel interlayer-confinement engineering strategy, utilizing spatially confined dual active sites in interlayerconfined dual single-atom-catalysts (iDSACs), to fundamentally break the intrinsic LSR by simultaneously manipulating reaction pathways and intermediate adsorption. Density functional theory (DFT) computations demonstrate that the synergistic space-electron effects enhance charge transfer, activate the O-O bond, and facilitate its dissociation. Further, tuning the confinement strength exerts opposing effects on various intermediates and catalysts. Consequently, this strategy effectively disrupts the LSR between *OOH and *OH adsorption, thereby improving OER and ORR activities. Additionally, an optimal interlayer distance of 7.0 & Aring; is identified to balance dual-site synergy and steric effects, achieving low overpotentials (0.26 V for OER and 0.30 V for ORR on IrN4). This work establishes space-electron synergy as a generic platform to disrupt adsorption scaling laws, advancing efficient electrocatalyst design and providing fundamental insights into confined electrocatalysis.