{"title":"鲁棒界面Ru中心高性能酸性氧演化","authors":"Xiaoju Cui, Pengju Ren, Chao Ma, Jia Zhao, Ruixue Chen, Shiming Chen, N. Pethan Rajan, Haobo Li, Liang Yu, Zhongqun Tian, Dehui Deng","doi":"10.1002/adma.201908126","DOIUrl":null,"url":null,"abstract":"<p>RuO<sub>2</sub> is considered as the state-of-the-art electrocatalyst for the oxygen evolution reaction (OER) in acidic media. However, its practical application is largely hindered by both the high reaction overpotential and severe electrochemical corrosion of the active centers. To overcome these limitations, innovative design strategies are necessary, which remains a great challenge. Herein, robust interface Ru centers between RuO<sub>2</sub> and graphene, via a controllable oxidation of graphene encapsulating Ru nanoparticles, are presented to efficiently enhance both the activity and stability of the acidic OER. Through precisely controlling the reaction interface, a much lower OER overpotential of only 227 mV at 10 mA cm<sup>−2</sup> in acidic electrolyte, compared with that of 290 mV for commercial RuO<sub>2</sub>, but a significantly higher durability than the commercial RuO<sub>2</sub>, are achieved. Density functional theory (DFT) calculations reveal that the interface Ru centers between the RuO<sub>2</sub> and the graphene can break the classic scaling relationships between the free energies of HOO* and HO* to reduce the limiting potential, rendering an enhancement in the intrinsic OER activity and the resistance to over-oxidation and corrosion for RuO<sub>2</sub>.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"32 25","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2020-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1002/adma.201908126","citationCount":"97","resultStr":"{\"title\":\"Robust Interface Ru Centers for High-Performance Acidic Oxygen Evolution\",\"authors\":\"Xiaoju Cui, Pengju Ren, Chao Ma, Jia Zhao, Ruixue Chen, Shiming Chen, N. Pethan Rajan, Haobo Li, Liang Yu, Zhongqun Tian, Dehui Deng\",\"doi\":\"10.1002/adma.201908126\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>RuO<sub>2</sub> is considered as the state-of-the-art electrocatalyst for the oxygen evolution reaction (OER) in acidic media. However, its practical application is largely hindered by both the high reaction overpotential and severe electrochemical corrosion of the active centers. To overcome these limitations, innovative design strategies are necessary, which remains a great challenge. Herein, robust interface Ru centers between RuO<sub>2</sub> and graphene, via a controllable oxidation of graphene encapsulating Ru nanoparticles, are presented to efficiently enhance both the activity and stability of the acidic OER. Through precisely controlling the reaction interface, a much lower OER overpotential of only 227 mV at 10 mA cm<sup>−2</sup> in acidic electrolyte, compared with that of 290 mV for commercial RuO<sub>2</sub>, but a significantly higher durability than the commercial RuO<sub>2</sub>, are achieved. Density functional theory (DFT) calculations reveal that the interface Ru centers between the RuO<sub>2</sub> and the graphene can break the classic scaling relationships between the free energies of HOO* and HO* to reduce the limiting potential, rendering an enhancement in the intrinsic OER activity and the resistance to over-oxidation and corrosion for RuO<sub>2</sub>.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":\"32 25\",\"pages\":\"\"},\"PeriodicalIF\":27.4000,\"publicationDate\":\"2020-05-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1002/adma.201908126\",\"citationCount\":\"97\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/adma.201908126\",\"RegionNum\":1,\"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":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.201908126","RegionNum":1,"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: 97
摘要
RuO2被认为是酸性介质中析氧反应(OER)最先进的电催化剂。然而,高反应过电位和活性中心严重的电化学腐蚀极大地阻碍了其实际应用。为了克服这些限制,创新的设计策略是必要的,这仍然是一个巨大的挑战。本文通过石墨烯包裹Ru纳米颗粒的可控氧化,在RuO2和石墨烯之间建立了强大的Ru中心界面,有效地提高了酸性OER的活性和稳定性。通过精确控制反应界面,在酸性电解液中,与商用RuO2的290 mV相比,在10 mA cm−2下,OER过电位仅为227 mV,但耐久性明显高于商用RuO2。密度泛函理论(DFT)计算表明,RuO2和石墨烯之间的界面Ru中心可以打破经典的HOO*和HO*自由能之间的标度关系,从而降低极限电位,从而增强RuO2的本征OER活性,增强其抗过氧化和耐腐蚀能力。
Robust Interface Ru Centers for High-Performance Acidic Oxygen Evolution
RuO2 is considered as the state-of-the-art electrocatalyst for the oxygen evolution reaction (OER) in acidic media. However, its practical application is largely hindered by both the high reaction overpotential and severe electrochemical corrosion of the active centers. To overcome these limitations, innovative design strategies are necessary, which remains a great challenge. Herein, robust interface Ru centers between RuO2 and graphene, via a controllable oxidation of graphene encapsulating Ru nanoparticles, are presented to efficiently enhance both the activity and stability of the acidic OER. Through precisely controlling the reaction interface, a much lower OER overpotential of only 227 mV at 10 mA cm−2 in acidic electrolyte, compared with that of 290 mV for commercial RuO2, but a significantly higher durability than the commercial RuO2, are achieved. Density functional theory (DFT) calculations reveal that the interface Ru centers between the RuO2 and the graphene can break the classic scaling relationships between the free energies of HOO* and HO* to reduce the limiting potential, rendering an enhancement in the intrinsic OER activity and the resistance to over-oxidation and corrosion for RuO2.
期刊介绍:
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