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Research Article

Layered double hydroxides with atomic-scale defects for superior electrocatalysis

Qixian Xie1,§Zhao Cai1,2,§Pengsong Li1Daojin Zhou1Yongmin Bi1Xuya Xiong1Enyuan Hu3Yaping Li1Yun Kuang1( )Xiaoming Sun1,4( )
State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing100029China
Department of Chemistry and Energy Sciences InstituteYale UniversityWest HavenConnecticut06516USA
Chemistry DivisionBrookhaven National Laboratory UptonNew York11973USA
College of EnergyBeijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing100029China

§ Qixian Xie and Zhao Cai contributed equally to this work.

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Abstract

Atomic composition tuning and defect engineering are effective strategies toenhance the catalytic performance of multicomponent catalysts by improvingthe synergetic effect; however, it remains challenging to dramatically tune the active sites on multicomponent materials through simultaneous defect engineeringat the atomic scale because of the similarities of the local environment. Herein, using the oxygen evolution reaction (OER) as a probe reaction, we deliberatelyintroduced base-soluble Zn(II) or Al(III) sites into NiFe layered double hydroxides(LDHs), which are one of the best OER catalysts. Then, the Zn(II) or Al(III) siteswere selectively etched to create atomic M(II)/M(III) defects, which dramaticallyenhanced the OER activity. At a current density of 20 mA·cm-2, only 200 mV overpotential was required to generate M(II) defect-rich NiFe LDHs, which is the best NiFe-based OER catalyst reported to date. Density functional theory(DFT) calculations revealed that the creation of dangling Ni–Fe sites (i.e., unsaturated coordinated Ni–Fe sites) by defect engineering of a Ni–O–Fe site at the atomic scale efficiently lowers the Gibbs free energy of the oxygen evolutionprocess. This defect engineering strategy provides new insights into catalysts atthe atomic scale and should be beneficial for the design of a variety of catalysts.

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Nano Research
Pages 4524-4534
Cite this article:
Xie Q, Cai Z, Li P, et al. Layered double hydroxides with atomic-scale defects for superior electrocatalysis. Nano Research, 2018, 11(9): 4524-4534. https://doi.org/10.1007/s12274-018-2033-9

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Received: 28 September 2017
Revised: 18 November 2017
Accepted: 24 February 2018
Published: 20 March 2018
© Tsinghua University Press and Springer‐Verlag GmbH Germany, part of Springer Nature 2018
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