Yong Feng, Huan Wang, Kun Feng, Chengyu Li, Shuo Li, Cheng Lu, Youyong Li, Ding Ma, Jun Zhong
{"title":"Atomic Manipulation to Create High-Valent Fe<sup>4+</sup> for Efficient and Ultrastable Oxygen Evolution at Industrial-Level Current Density.","authors":"Yong Feng, Huan Wang, Kun Feng, Chengyu Li, Shuo Li, Cheng Lu, Youyong Li, Ding Ma, Jun Zhong","doi":"10.1021/acsnano.4c09259","DOIUrl":null,"url":null,"abstract":"<p><p>Manipulating the electronic structure of a catalyst at the atomic level is an effective but challenging way to improve the catalytic performance. Here, by stretching the Fe-O bond in FeOOH with an inserted Mo atom, a Fe-O-Mo unit can be created, which will induce the formation of high-valent Fe<sup>4+</sup> during the alkaline oxygen evolution reaction (OER). The highly active Fe<sup>4+</sup> state has been clearly revealed by in situ X-ray absorption spectroscopy, which can both enhance the oxidation capability and lead to an efficient and stable adsorbate evolution mechanism (AEM) pathway for the OER. As a result, the obtained Fe-Mo-Ni<sub>3</sub>S<sub>2</sub> catalyst exhibits both superior OER activity and outstanding stability, which can achieve an industrial-level current density of 1 A cm<sup>-2</sup> at a low overpotential of 259 mV (at 60 °C) and can stably work at the large current for more than 2000 h. Moreover, by coupling with commercial Pt/C, the Fe-Mo-Ni<sub>3</sub>S<sub>2</sub>∥Pt/C system can be used in the anion exchange membrane cell to acquire 1 A cm<sup>-2</sup> for overall water splitting at 1.68 V (2.03 V for 4 A cm<sup>-2</sup>), outperforming the benchmark RuO<sub>2</sub>∥Pt/C system. The efficient, low-cost, and ultrastable OER catalyst enabled by manipulating the atomic structure may provide potential opportunities for future practical water splitting.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":null,"pages":null},"PeriodicalIF":15.8000,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsnano.4c09259","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/10/10 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Manipulating the electronic structure of a catalyst at the atomic level is an effective but challenging way to improve the catalytic performance. Here, by stretching the Fe-O bond in FeOOH with an inserted Mo atom, a Fe-O-Mo unit can be created, which will induce the formation of high-valent Fe4+ during the alkaline oxygen evolution reaction (OER). The highly active Fe4+ state has been clearly revealed by in situ X-ray absorption spectroscopy, which can both enhance the oxidation capability and lead to an efficient and stable adsorbate evolution mechanism (AEM) pathway for the OER. As a result, the obtained Fe-Mo-Ni3S2 catalyst exhibits both superior OER activity and outstanding stability, which can achieve an industrial-level current density of 1 A cm-2 at a low overpotential of 259 mV (at 60 °C) and can stably work at the large current for more than 2000 h. Moreover, by coupling with commercial Pt/C, the Fe-Mo-Ni3S2∥Pt/C system can be used in the anion exchange membrane cell to acquire 1 A cm-2 for overall water splitting at 1.68 V (2.03 V for 4 A cm-2), outperforming the benchmark RuO2∥Pt/C system. The efficient, low-cost, and ultrastable OER catalyst enabled by manipulating the atomic structure may provide potential opportunities for future practical water splitting.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.