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孤立八面体铂诱导电子转移至超低含量钌掺杂的尖晶石氧化钴以增强酸性全水分解性能

Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel CoO for Enhanced Acidic Overall Water Splitting.

作者信息

Li Di, Xu Danyun, Pei Yuhou, Zhang Qicheng, Lu Yingying, Zhang Bing

机构信息

State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.

ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China.

出版信息

J Am Chem Soc. 2024 Oct 23;146(42):28728-28738. doi: 10.1021/jacs.4c07089. Epub 2024 Sep 13.

Abstract

The development of a highly active and stable oxygen evolution reaction (OER) electrocatalyst is desirable for sustainable and efficient hydrogen production via proton exchange membrane water electrolysis (PEMWE) powered by renewable electricity yet challenging. Herein, we report a robust Pt/Ru-codoped spinel cobalt oxide (PtRu-CoO) electrocatalyst with an ultralow precious metal loading for acidic overall water splitting. PtRu-CoO exhibits excellent catalytic activity (1.63 V at 100 mA cm) and outstanding stability without significant performance degradation for 100 h operation. Experimental analysis and theoretical calculations indicate that Pt doping can induce electron transfer to Ru-doped CoO, optimize the absorption energy of oxygen intermediates, and stabilize metal-oxygen bonds, thus enhancing the catalytic performance through an adsorbate-evolving mechanism. As a consequence, the PEM electrolyzer featuring PtRu-CoO catalyst with low precious metal mass loading of 0.23 mg cm can drive a current density of 1.0 A cm at 1.83 V, revealing great promise for the application of noniridium-based catalysts with low contents of precious metal for hydrogen production.

摘要

开发一种高活性且稳定的析氧反应(OER)电催化剂对于通过可再生电力驱动的质子交换膜水电解(PEMWE)实现可持续且高效的制氢而言是很有必要的,但却具有挑战性。在此,我们报道了一种用于酸性全水解的超低贵金属负载量的稳健的铂/钌共掺杂尖晶石钴氧化物(PtRu-CoO)电催化剂。PtRu-CoO表现出优异的催化活性(100 mA cm²时为1.63 V)以及出色的稳定性,在运行100小时后性能无显著下降。实验分析和理论计算表明,铂掺杂可诱导电子转移至钌掺杂的CoO,优化氧中间体的吸附能,并稳定金属-氧键,从而通过吸附质演化机制提高催化性能。因此,采用PtRu-CoO催化剂、贵金属质量负载量低至0.23 mg cm²的PEM电解槽在1.83 V时可驱动1.0 A cm²的电流密度,这表明低贵金属含量的非铱基催化剂在制氢应用方面具有巨大潜力。

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