{"title":"利用导电 Ti4O7 支持物促进低r 催化水氧化的界面工程策略","authors":"Yufeng Qin, Yifan Wang, Rou Wen, Longxiang Wang, Meiling Dou, Feng Wang","doi":"10.1021/acscatal.4c03862","DOIUrl":null,"url":null,"abstract":"The need to use expensive and scarce Ir-based catalysts in the oxygen evolution reaction (OER) hinders the large-scale application of proton exchange membrane water electrolysis (PEMWE). Herein, we present an effective interface-engineering strategy to boost the efficacy of low-Ir catalysis of OER by means of electron transfer and lattice oxygen stabilization at the catalyst–support interface by utilizing a highly conductive (∼960 S cm<sup>–1</sup>) Ti<sub>4</sub>O<sub>7</sub> support to strongly anchor IrO<sub>2</sub> nanoparticles. Experimental and theoretical calculations suggest that Ti<sub>4</sub>O<sub>7</sub> tailors the Ir electronic structure that results from the formation of Ir–O–Ti bonds at the IrO<sub>2</sub>–Ti<sub>4</sub>O<sub>7</sub> interface, resulting in a lowered d-band center that weakens the adsorption of oxygen intermediates on Ir sites and thus boosts OER catalysis. The Ir–O–Ti bonds formed at the interface stabilize lattice oxygen in IrO<sub>2</sub>, facilitating a stable lattice oxygen mechanism path for OER catalysis. The interface effect results in superior OER activity with an overpotential of 244 mV at 10 mA cm<sup>–2</sup> and a high mass activity of 1342.9 A g<sub>Ir</sub><sup>–1</sup> (93.25× that of commercial IrO<sub>2</sub>), and the material also shows better durability than commercial IrO<sub>2</sub>. This interface-engineering strategy affords a strong catalyst–support interaction and should facilitate the design of high-performance catalysts for PEMWE applications.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":11.3000,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Interface-Engineering Strategy for Boosting Low-Ir Catalytic Water Oxidation Using a Conductive Ti4O7 Support\",\"authors\":\"Yufeng Qin, Yifan Wang, Rou Wen, Longxiang Wang, Meiling Dou, Feng Wang\",\"doi\":\"10.1021/acscatal.4c03862\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The need to use expensive and scarce Ir-based catalysts in the oxygen evolution reaction (OER) hinders the large-scale application of proton exchange membrane water electrolysis (PEMWE). Herein, we present an effective interface-engineering strategy to boost the efficacy of low-Ir catalysis of OER by means of electron transfer and lattice oxygen stabilization at the catalyst–support interface by utilizing a highly conductive (∼960 S cm<sup>–1</sup>) Ti<sub>4</sub>O<sub>7</sub> support to strongly anchor IrO<sub>2</sub> nanoparticles. Experimental and theoretical calculations suggest that Ti<sub>4</sub>O<sub>7</sub> tailors the Ir electronic structure that results from the formation of Ir–O–Ti bonds at the IrO<sub>2</sub>–Ti<sub>4</sub>O<sub>7</sub> interface, resulting in a lowered d-band center that weakens the adsorption of oxygen intermediates on Ir sites and thus boosts OER catalysis. The Ir–O–Ti bonds formed at the interface stabilize lattice oxygen in IrO<sub>2</sub>, facilitating a stable lattice oxygen mechanism path for OER catalysis. The interface effect results in superior OER activity with an overpotential of 244 mV at 10 mA cm<sup>–2</sup> and a high mass activity of 1342.9 A g<sub>Ir</sub><sup>–1</sup> (93.25× that of commercial IrO<sub>2</sub>), and the material also shows better durability than commercial IrO<sub>2</sub>. This interface-engineering strategy affords a strong catalyst–support interaction and should facilitate the design of high-performance catalysts for PEMWE applications.\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2024-09-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acscatal.4c03862\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c03862","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
氧进化反应(OER)需要使用昂贵而稀缺的铱基催化剂,这阻碍了质子交换膜电解水(PEMWE)的大规模应用。在此,我们提出了一种有效的界面工程策略,利用高导电性(∼ 960 S cm-1)的 Ti4O7 载体强力锚定 IrO2 纳米粒子,通过催化剂-载体界面的电子转移和晶格氧稳定,提高低铁催化 OER 的功效。实验和理论计算表明,Ti4O7 可调整 IrO2-Ti4O7 界面形成的 Ir-O-Ti 键所产生的 Ir 电子结构,从而降低 d 带中心,减弱氧中间体对 Ir 位点的吸附,从而促进 OER 催化。在界面上形成的 Ir-O-Ti 键稳定了 IrO2 中的晶格氧,为 OER 催化提供了稳定的晶格氧机制路径。界面效应产生了卓越的OER活性,在10 mA cm-2条件下过电位为244 mV,质量活性高达1342.9 A gIr-1(是商用IrO2的93.25倍),而且该材料的耐久性也优于商用IrO2。这种界面工程策略提供了催化剂与支撑物之间的强相互作用,应有助于设计用于 PEMWE 应用的高性能催化剂。
Interface-Engineering Strategy for Boosting Low-Ir Catalytic Water Oxidation Using a Conductive Ti4O7 Support
The need to use expensive and scarce Ir-based catalysts in the oxygen evolution reaction (OER) hinders the large-scale application of proton exchange membrane water electrolysis (PEMWE). Herein, we present an effective interface-engineering strategy to boost the efficacy of low-Ir catalysis of OER by means of electron transfer and lattice oxygen stabilization at the catalyst–support interface by utilizing a highly conductive (∼960 S cm–1) Ti4O7 support to strongly anchor IrO2 nanoparticles. Experimental and theoretical calculations suggest that Ti4O7 tailors the Ir electronic structure that results from the formation of Ir–O–Ti bonds at the IrO2–Ti4O7 interface, resulting in a lowered d-band center that weakens the adsorption of oxygen intermediates on Ir sites and thus boosts OER catalysis. The Ir–O–Ti bonds formed at the interface stabilize lattice oxygen in IrO2, facilitating a stable lattice oxygen mechanism path for OER catalysis. The interface effect results in superior OER activity with an overpotential of 244 mV at 10 mA cm–2 and a high mass activity of 1342.9 A gIr–1 (93.25× that of commercial IrO2), and the material also shows better durability than commercial IrO2. This interface-engineering strategy affords a strong catalyst–support interaction and should facilitate the design of high-performance catalysts for PEMWE applications.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.