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Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel Co3O4 for Enhanced Acidic Overall Water Splitting
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-09-13 , DOI: 10.1021/jacs.4c07089
Di Li 1, 2 , Danyun Xu 3, 4 , Yuhou Pei 1, 2 , Qicheng Zhang 3 , Yingying Lu 1, 2 , Bing Zhang 1, 2
Affiliation  

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–Co3O4) electrocatalyst with an ultralow precious metal loading for acidic overall water splitting. PtRu–Co3O4 exhibits excellent catalytic activity (1.63 V at 100 mA cm–2) 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 Co3O4, 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–Co3O4 catalyst with low precious metal mass loading of 0.23 mg cm–2 can drive a current density of 1.0 A cm–2 at 1.83 V, revealing great promise for the application of noniridium-based catalysts with low contents of precious metal for hydrogen production.

中文翻译:


孤立八面体 Pt 诱导电子转移至超低含量钌掺杂尖晶石 Co3O4,用于增强酸性整体水分解



开发高活性和稳定的析氧反应(OER)电催化剂对于通过由可再生电力驱动的质子交换膜水电解(PEMWE)可持续和高效地生产氢气来说是可取的,但也具有挑战性。在此,我们报道了一种坚固的 Pt/Ru 共掺杂尖晶石钴氧化物 (PtRu–Co 3 O 4 ) 电催化剂,具有超低的贵金属负载量,用于酸性整体水分解。 PtRu–Co 3 O 4表现出优异的催化活性(100 mA cm –2时为 1.63 V)和出色的稳定性,运行 100 小时不会出现明显的性能下降。实验分析和理论计算表明,Pt掺杂可以诱导电子转移到Ru掺杂的Co 3 O 4 ,优化氧中间体的吸收能,稳定金属-氧键,从而通过吸附质演化机制增强催化性能。因此,采用PtRu–Co 3 O 4催化剂且贵金属质量负载量低至0.23 mg cm –2的PEM电解槽可以在1.83 V下驱动1.0 A cm –2的电流密度,为非铱的应用展现了巨大的前景。用于制氢的低贵金属含量的催化剂。
更新日期:2024-09-17
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