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半金属氢氧化物材料用于电化学水氧化

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寻找具有高本征活性的水氧化催化剂材料对许多清洁能源技术的发展至关重要.氢氧化物半导体对析氧反应具有一定的电催化活性.然而,该材料导电性较差,限制着其电催化本征活性的提升.本文提出一种兼具高导电性和高催化活性的半金属氢氧化物析氧电催化材料.通过阳离子掺杂和阴离子空位协同作用,镍铁水滑石半导体可转化为半金属材料,其电阻率降低了两个数量级.相应半金属氢氧化物阵列电极的电催化活性显著提升,在10 mA cm-2电流密度下其析氧过电势仅为195mV,Tafel斜率仅为40.9 mV dec-1,显著优于商用RuO2催化剂(316 mV,99.6 mV dec-1).原位拉曼光谱和理论计算结果表明,半金属氢氧化物可在较低过电位下转化为羟基氧化物中间体,有助于高价态金属活性位点的形成与稳定,从而提升材料的析氧本征活性.本研究表明,兼具优异导电性和催化活性的半金属氢氧化物可作为先进的电极材料.
Semimetallic hydroxide materials for electrochemical water oxidation
Searching for catalyst materials with high in-trinsic activity for water oxidation holds the key to numerous clean energy technologies.Hydroxide semiconductors are electrochemically active to drive oxygen evolution reaction(OER),but suffer from poor electronic conductivity,restrict-ing their intrinsic electrocatalytic activity.Here,a semi-metallic hydroxide material was designed as efficient OER catalyst with both improved electronic conductivity and in-trinsic electrocatalytic activity.By cationic doping and anionic vacancy manipulation,the NiFe layered double hydroxide(LDH)semiconductor was turned into semi-metallic with two orders of magnitude lower resistivity.Consequently,the semi-metallic LDH(SM LDH)array electrode exhibited an in-trinsically improved OER activity with a low overpotential of 195 mV at 10 mA cm-2 and a low Tafel slope of 40.9 mV dec-1 in alkaline medium,outperforming commercial RuO2 cata-lysts(316 mV,99.6 mV dec-1)under the same test condition.In-depth Raman and first-principles calculations demon-strated that the enhanced OER intrinsic activity of SM LDH was associated with the high electronic conductivity,which promoted the formation and stabilization of high-valence metal sites in oxyhydroxide intermediates.These finding suggest semi-metallic hydroxides as an advanced electrode material with both fascinating electric and catalytic properties.

electrocatalysthydroxidesemi-metalelectric con-ductivityintrinsic activity

王静、Mohammed-Ibrahim Jamesh、高强、韩波、孙睿敏、Hsien-Yi Hsu、周成冈、蔡钊

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Faculty of Materials Science and Chemistry,China University of Geosciences,Wuhan 430074,China

School of Energy and Environment,Department of Materials Science and Engineering,City University of Hong Kong,Kowloon Tong,Hong Kong 999077,China

electrocatalyst hydroxide semi-metal electric con-ductivity intrinsic activity

National Natural Science Foundation of ChinaNational Natural Science Foundation of Chinathe"CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)Fundamental Research Funds for the Central Universities,China University of Geosciences(Wuhan)

22205068221091442022118162301202673

2024

10.1007/s40843-023-2802-8

中国科学:材料科学(英文)

中国科学:材料科学(英文)

CSTPCD
ISSN：
年,卷(期)：2024.67(5)
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