Fei Wu, Biao Wu, Liang Chen, Yunan Wang, Jiejie Li and Qiuju Zhang
{"title":"通过调节不对称多位点 NiOOH 探索双位点 OER 机制","authors":"Fei Wu, Biao Wu, Liang Chen, Yunan Wang, Jiejie Li and Qiuju Zhang","doi":"10.1039/D4NR01869A","DOIUrl":null,"url":null,"abstract":"<p >Asymmetric nickel oxyhydroxide (NiOOH) possesses multi-OH and O active sites on different surfaces, (001) and (00<img>), which possibly causes a complicated catalytic process. Density functional theory (DFT) calculations reveal that the unconventional dual-site mechanism (UDSM) of the oxygen evolution reaction (OER) on NiOOH (001) and (00<img>) exhibits significantly lower overpotentials of 0.80 and 0.77 V, compared to 1.24 and 1.62 V for the single-site mechanism (SSM), respectively. Through chemical doping or heterojunction modifications, the constructed NiOOH@FeOOH (00<img>) heterojunction reduces the thermodynamic overpotential to 0.49 V from original 0.77 V undergoing the UDSM. Although Fe/Co-doping or physical compression yield similar or slightly higher overpotentials and are not conductive to facilitating the OER process by the UDSM, all dual-site paths exhibit obviously lower overpotentials than the SSM for pristine and regulated NiOOH (001) and (00<img>) from the whole viewpoint. This work identifies a more reasonable and efficient dual-site OER mechanism, which is expected to help the rational design of highly-efficient electrocatalysts.</p>","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Dual-site OER mechanism exploration through regulating asymmetric multi-site NiOOH†\",\"authors\":\"Fei Wu, Biao Wu, Liang Chen, Yunan Wang, Jiejie Li and Qiuju Zhang\",\"doi\":\"10.1039/D4NR01869A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Asymmetric nickel oxyhydroxide (NiOOH) possesses multi-OH and O active sites on different surfaces, (001) and (00<img>), which possibly causes a complicated catalytic process. Density functional theory (DFT) calculations reveal that the unconventional dual-site mechanism (UDSM) of the oxygen evolution reaction (OER) on NiOOH (001) and (00<img>) exhibits significantly lower overpotentials of 0.80 and 0.77 V, compared to 1.24 and 1.62 V for the single-site mechanism (SSM), respectively. Through chemical doping or heterojunction modifications, the constructed NiOOH@FeOOH (00<img>) heterojunction reduces the thermodynamic overpotential to 0.49 V from original 0.77 V undergoing the UDSM. Although Fe/Co-doping or physical compression yield similar or slightly higher overpotentials and are not conductive to facilitating the OER process by the UDSM, all dual-site paths exhibit obviously lower overpotentials than the SSM for pristine and regulated NiOOH (001) and (00<img>) from the whole viewpoint. This work identifies a more reasonable and efficient dual-site OER mechanism, which is expected to help the rational design of highly-efficient electrocatalysts.</p>\",\"PeriodicalId\":92,\"journal\":{\"name\":\"Nanoscale\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-06-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nanoscale\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/nr/d4nr01869a\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanoscale","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/nr/d4nr01869a","RegionNum":3,"RegionCategory":"材料科学","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
不对称氢氧化镍(NiOOH)在不同的表面(001)和(001 @#x0305;)上具有多个OH和O活性位点,这可能会导致复杂的催化过程。密度泛函理论(DFT)计算显示,NiOOH(001)和(001 @#x0305;)表面氧进化反应的非常规双位点机理(UDSM)的过电势分别为 0.80 V 和 0.77 V,明显低于单位点机理(SSM)的 1.24 V 和 1.62 V。通过化学掺杂或异质结修饰,所构建的 NiOOH@FeOOH (001 @#x0305;) 异质结将 UDSM 的热力学过电位从原来的 0.77 V 降低到 0.49 V。虽然铁/钴掺杂或物理压缩产生的过电位相近或略高,而且对促进 UDSM 的 OER 过程没有传导作用,但从整体上看,对于原始和调节的 NiOOH (001) 和 (001 @#x0305;),所有双位点路径都表现出明显低于 SSM 的过电位。这项研究发现了一种更合理、更高效的双位点 OER 机制,有望帮助合理设计高效电催化剂。
Dual-site OER mechanism exploration through regulating asymmetric multi-site NiOOH†
Asymmetric nickel oxyhydroxide (NiOOH) possesses multi-OH and O active sites on different surfaces, (001) and (00), which possibly causes a complicated catalytic process. Density functional theory (DFT) calculations reveal that the unconventional dual-site mechanism (UDSM) of the oxygen evolution reaction (OER) on NiOOH (001) and (00) exhibits significantly lower overpotentials of 0.80 and 0.77 V, compared to 1.24 and 1.62 V for the single-site mechanism (SSM), respectively. Through chemical doping or heterojunction modifications, the constructed NiOOH@FeOOH (00) heterojunction reduces the thermodynamic overpotential to 0.49 V from original 0.77 V undergoing the UDSM. Although Fe/Co-doping or physical compression yield similar or slightly higher overpotentials and are not conductive to facilitating the OER process by the UDSM, all dual-site paths exhibit obviously lower overpotentials than the SSM for pristine and regulated NiOOH (001) and (00) from the whole viewpoint. This work identifies a more reasonable and efficient dual-site OER mechanism, which is expected to help the rational design of highly-efficient electrocatalysts.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.