Structural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO₂ substrate supported CoS_1.97 (CeO₂-CoS_1.97) and CoS_1.97 with CeO₂ surface decorated (CoS_1.97-CeO₂) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER). CeO₂-CoS_1.97 exhibits a low overpotential of 264 mV at 10 mA cm⁻² due to the stable heterostructure and faster mass transfer. Meanwhile, CoS_1.97-CeO₂ has a smaller Tafel slope of 49 mV dec⁻¹ through enhanced adsorption of OH⁻, fast electron transfer, and in situ formation of Co(IV)O₂ species under the OER condition. Furthermore, operando spectroscopic characterizations combined with theoretical calculations demonstrate that spatial architectures play a distinguished role in modulating the electronic structure and promoting the reconstruction from sulfide to oxyhydroxide toward higher chemical valence. The findings highlight spatial architectures and surface reconstruction in designing advanced electrocatalytic materials.

中文翻译：

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揭示具有特定空间结构的 CeO2/CoS1.97 异质结构对氧释放反应的促进作用

结构工程和成分控制广泛应用于合理设计和制造先进的独立式电催化剂。组分的空间分布与增强的电催化性能之间的关键关系仍有待进一步阐明。在此，铈₂衬底支撑的CoS _1.97（的CeO ₂ -cos _1.97）和CoS _1.97用的CeO ₂表面装饰等级（CoS _1.97 -CeO ₂）的材料被构造成全面调查的析氧反应（OER）的空间架构的起源。CeO ₂ -CoS _1.97由于稳定的异质结构和更快的传质，在 10 mA cm ^{-2 下}表现出 264 mV 的低过电位。同时，CoS _1.97 -CeO ₂通过增强OH ^{- 的}吸附、快速电子转移和Co(IV)O _{2 的}原位形成而具有较小的Tafel 斜率49 mV dec ^-1OER 条件下的物种。此外，操作光谱表征与理论计算相结合表明，空间结构在调节电子结构和促进从硫化物到羟基氧化物向更高化学价的重建方面发挥着显着的作用。研究结果突出了设计先进电催化材料的空间结构和表面重建。