Synergistic interlayer confinement and built-in electric field construct reconstruction-inhibited cobalt selenide for robust oxygen evolution at high current density

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters Pub Date : 2025-06-11 DOI:10.1016/j.cclet.2025.111441

Yuanhua Xiao , Jinhui Shou , Shiwei Zhang , Ya Shen , Junwei Liu , Dangcheng Su , Yang Kong , Xiaodong Jia , Qingxiang Yang , Shaoming Fang , Xuezhao Wang

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Abstract

Transition metal selenides (TMS) demonstrate exceptional catalytic activity in the oxygen evolution reaction (OER), yet their performance is hindered by surface reconstruction under OER conditions, particularly at high current densities. This study reveals that embedding Co_0.85Se nanoparticles into the interlayer spacing of MXene-Ti₃C₂ effectively suppresses surface reconstruction during OER. This configuration establishes a Schottky heterojunction with an intrinsic built-in electric field (BEF) between Co_0.85Se and Ti₃C₂, which enhances charge redistribution and accelerates electron transport. Consequently, the Co_0.85Se@Ti₃C₂ composite exhibits outstanding OER performance, achieving low overpotentials (230 mV at 100 mA/cm², 376 mV at 1000 mA/cm², 417 mV at 1500 mA/cm²) and exceptional durability (200 h at 200 mA/cm²). In-situ XRD/Raman characterization verifies that the encapsulated Co_0.85Se within Ti₃C₂ inhibits CoOOH formation on the surface during OER. Both experimental and theoretical investigations indicate that the heterojunction's superhydrophilicity/superaerophobicity, synergized with BEF-regulated oxygen intermediate adsorption/desorption, collectively enhance catalytic efficiency of Co_0.85Se@Ti₃C₂. This strategy of spatially confining chalcogenide catalysts to prevent structural degradation while leveraging interfacial electric fields presents a rational approach for developing durable electrocatalysts in high-current densities water electrolysis.

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协同层间约束和内置电场构建重建抑制硒化钴在高电流密度下的稳健析氧

过渡金属硒化物（TMS）在析氧反应（OER）中表现出优异的催化活性，但在OER条件下，特别是在高电流密度下，其性能受到表面重构的阻碍。研究表明，在MXene-Ti3C2的层间嵌入Co0.85Se纳米粒子可以有效抑制OER过程中的表面重建。这种构型在Co0.85Se和Ti3C2之间建立了具有本征内建电场（BEF）的肖特基异质结，增强了电荷的再分配，加速了电子的传递。因此,Co0.85Se@Ti3C2复合展品突出OER性能,实现过电压低(230年 mV 100 mA / cm2, 376 mV在1000 mA / cm2, 417 mV 1500 mA / cm2)和特殊的耐久性(200 h 200 mA / cm2)。原位XRD/Raman表征证实，包封在Ti3C2内的Co0.85Se抑制了OER过程中表面CoOOH的形成。实验和理论研究表明，异质结的超亲水性/超疏水性与bef调节的氧中间体吸附/解吸协同作用，共同提高了Co0.85Se@Ti3C2的催化效率。这种在空间上限制硫系催化剂以防止结构降解，同时利用界面电场的策略为开发高电流密度水电解中耐用的电催化剂提供了一种合理的方法。

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来源期刊

Chinese Chemical Letters 化学-化学综合

CiteScore

14.10

自引率

15.40%

发文量

8969

审稿时长

1.6 months

期刊介绍： Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.