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

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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：

孤立的八面体 Pt 诱导电子转移至超低含量的钌掺杂尖晶石 Co3O4 以增强酸性整体水分解

开发一种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提供动力的质子交换膜水电解（PEMWE）进行可持续和高效的制氢是理想的，但具有挑战性。在本文中，我们报道了一种稳定的 Pt/Ru 共掺杂尖晶石钴氧化物（PtRu–Co₃O₄）电催化剂，具有超低贵金属负载量，适用于酸性整体水分解。PtRu–Co₃O₄ 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，在 100 h 运行中性能不会显著下降。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 Co₃O₄ 上，优化氧中间体的吸收能，稳定金属-氧键，从而通过析出吸附物机制增强催化性能。因此，采用 PtRu-Co₃O₄ 催化剂的 PEM 电解槽具有 0.23 mg cm^–2 的低贵金属质量负载，可以在 1.83 V 下驱动 1.0 A cm^–2 的电流密度，为低贵金属含量的壬铱基催化剂在制氢中的应用带来了巨大的前景。

更新日期：2024-09-13

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