{"title":"隔离八面体铂诱导电子转移到超低含量钌掺杂尖晶石 Co3O4 以增强酸性整体水分离效果","authors":"Di Li, Danyun Xu, Yuhou Pei, Qicheng Zhang, Yingying Lu, Bing Zhang","doi":"10.1021/jacs.4c07089","DOIUrl":null,"url":null,"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–Co<sub>3</sub>O<sub>4</sub>) electrocatalyst with an ultralow precious metal loading for acidic overall water splitting. PtRu–Co<sub>3</sub>O<sub>4</sub> exhibits excellent catalytic activity (1.63 V at 100 mA cm<sup>–2</sup>) 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 Co<sub>3</sub>O<sub>4</sub>, 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–Co<sub>3</sub>O<sub>4</sub> catalyst with low precious metal mass loading of 0.23 mg cm<sup>–2</sup> can drive a current density of 1.0 A cm<sup>–2</sup> at 1.83 V, revealing great promise for the application of noniridium-based catalysts with low contents of precious metal for hydrogen production.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel Co3O4 for Enhanced Acidic Overall Water Splitting\",\"authors\":\"Di Li, Danyun Xu, Yuhou Pei, Qicheng Zhang, Yingying Lu, Bing Zhang\",\"doi\":\"10.1021/jacs.4c07089\",\"DOIUrl\":null,\"url\":null,\"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–Co<sub>3</sub>O<sub>4</sub>) electrocatalyst with an ultralow precious metal loading for acidic overall water splitting. PtRu–Co<sub>3</sub>O<sub>4</sub> exhibits excellent catalytic activity (1.63 V at 100 mA cm<sup>–2</sup>) 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 Co<sub>3</sub>O<sub>4</sub>, 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–Co<sub>3</sub>O<sub>4</sub> catalyst with low precious metal mass loading of 0.23 mg cm<sup>–2</sup> can drive a current density of 1.0 A cm<sup>–2</sup> at 1.83 V, revealing great promise for the application of noniridium-based catalysts with low contents of precious metal for hydrogen production.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-09-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c07089\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c07089","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
开发一种高活性、高稳定性的氧进化反应(OER)电催化剂是利用可再生电力通过质子交换膜电解水(PEMWE)实现可持续高效制氢的理想选择,但这一研究仍具有挑战性。在此,我们报告了一种具有超低贵金属负载的强效铂/钌掺杂尖晶石氧化钴(PtRu-Co3O4)电催化剂,可用于酸性整体水分离。PtRu-Co3O4 表现出卓越的催化活性(100 mA cm-2 时为 1.63 V)和出色的稳定性,在 100 小时的运行过程中不会出现明显的性能衰减。实验分析和理论计算表明,掺杂铂能诱导电子转移到掺Ru的Co3O4上,优化氧中间产物的吸收能量,稳定金属氧键,从而通过吸附剂进化机制提高催化性能。因此,采用铂钌钴氧化物(PtRu-Co3O4)催化剂的 PEM 电解槽在 1.83 V 电压下可驱动 1.0 A cm-2 的电流密度,贵金属含量低的非铱基催化剂在制氢领域的应用前景广阔。
Isolated Octahedral Pt-Induced Electron Transfer to Ultralow-Content Ruthenium-Doped Spinel Co3O4 for Enhanced Acidic Overall Water Splitting
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.
期刊介绍:
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