Surface Nanosteps Modulate the Local Environment of Co Single Atoms to Boost the Electrocatalytic Hydrogen Evolution Reaction

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-12-07 DOI:10.1021/acscatal.4c0562410.1021/acscatal.4c05624

Sheng Qian, Tengfei Jiang*, Junhua Wang, Wenzhi Yuan, Dailing Jia, Ningyan Cheng, Huaiguo Xue, Zhongfei Xu*, Romain Gautier* and Jingqi Tian*,

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Abstract

Modulating the coordination environment of non-noble-metal single-atom catalysts is of great significance to boost their catalytic performance. However, the outcome of this approach strongly relies on the structural design of the support. Herein, we demonstrate that nanosteps on titanium oxide, which can be simply generated by HCl etching, enable regulation of the coordination environment of anchored Co single atoms. Thus, experimental and theoretical results revealed that nanostepped TiO₂ selectively anchors three-coordinated Co–P₃ on the step-edge, while flat TiO₂ supports four-coordinated Co–P₃O. These Co–P₃ sites demonstrate significantly enhanced hydrogen evolution reaction (HER) performance, achieving a mass activity approximately 8.3 times greater than that of the Co–P₃O on flat TiO₂. The unsaturated step-edge configuration of TiO₂ induces more electron transfer from the support to Co–P₃ through the Ti–P–Co pathway. This electron accumulation is further amplified by the electric field effect induced by nanosteps and optimizes the energy required for H₂O dissociation and OH*/H* adsorption and desorption during the electrocatalytic HER.

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表面纳米步调节Co单原子局部环境促进电催化析氢反应

调节非贵金属单原子催化剂的配位环境对提高其催化性能具有重要意义。然而，这种方法的结果在很大程度上取决于载体的结构设计。在此，我们证明了通过盐酸蚀刻就能简单生成的氧化钛纳米阶梯能够调节锚定钴单原子的配位环境。因此，实验和理论结果表明，纳米阶梯状氧化钛可选择性地在阶梯边缘锚定三配位 Co-P3，而平面氧化钛则支持四配位 Co-P3O。这些 Co-P3 位点显著增强了氢进化反应（HER）性能，其质量活性是平面二氧化钛上 Co-P3O 的约 8.3 倍。二氧化钛的不饱和阶梯边构型促使更多的电子通过 Ti-P-Co 途径从支撑物转移到 Co-P3。纳米阶梯诱导的电场效应进一步扩大了电子积累，优化了电催化 HER 过程中 H2O 解离和 OH*/H* 吸附与解吸所需的能量。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.