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钴基电催化剂在水氧化中的强表面亲水性。

Strong Surface Hydrophilicity in Co-Based Electrocatalysts for Water Oxidation.

机构信息

National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei 230029, Anhui, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2017 Aug 16;9(32):26867-26873. doi: 10.1021/acsami.7b07088. Epub 2017 Aug 4.

Abstract

Developing efficient and durable oxygen evolution electrocatalyst is of paramount importance for the large-scale supply of renewable energy sources. Herein, we report the design of significant surface hydrophilicity based on cobalt oxyhydroxide (CoOOH) nanosheets to greatly improve the surface hydroxyl species adsorption and reaction kinetics at the Helmholtz double layer for high-efficiency water oxidation activity. The as-designed CoOOH-graphene nanosheets achieve a small surface water contact angle of ∼23° and a large double-layer capacitance (C) of 8.44 mF/cm and thus could evidently strengthen surface species adsorption and trigger electrochemical oxygen evolution reaction (OER) under a quite low onset potential of 200 mV with an excellent Tafel slope of 32 mV/dec. X-ray absorption spectroscopy and first-principles calculations demonstrate that the strong interface electron coupling between CoOOH and graphene extracts partial electrons from the active sties and increases the electron state density around the Fermi level and effectively promotes the surface intermediates formation for efficient OER.

摘要

开发高效、持久的氧析出电催化剂对于可再生能源的大规模供应至关重要。在此,我们报告了基于钴氢氧化物(CoOOH)纳米片的显著表面亲水性设计,以极大地提高亥姆霍兹双电层中表面羟基物种的吸附和反应动力学,从而实现高效水氧化活性。所设计的 CoOOH-石墨烯纳米片具有约 23°的小表面水接触角和 8.44 mF/cm 的大双层电容(C),因此可以明显增强表面物种的吸附,并在相当低的起始电位 200 mV 下引发电化学氧析出反应(OER),具有优异的 32 mV/dec 的塔菲尔斜率。X 射线吸收光谱和第一性原理计算表明,CoOOH 和石墨烯之间的强界面电子耦合从活性位点提取部分电子,并增加费米能级附近的电子态密度,从而有效促进表面中间产物的形成,实现高效的 OER。

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