Layered double hydroxides with atomic-scale defects for superior electrocatalysis

Xie, Qixian; Cai, Zhao; Li, Pengsong; Zhou, Daojin; Bi, Yongmin; Xiong, Xuya; Hu, Enyuan; Li, Yaping; Kuang, Yun; Sun, Xiaoming

doi:10.1007/s12274-018-2033-9

Layered double hydroxides with atomic-scale defects for superior electrocatalysis

Journal Article · Tue Mar 20 00:00:00 EDT 2018 · Nano Research

DOI:https://doi.org/10.1007/s12274-018-2033-9· OSTI ID:1473662

Xie, Qixian ^[1]; Cai, Zhao ^[2]; Li, Pengsong ^[1]; Zhou, Daojin ^[1]; Bi, Yongmin ^[1]; Xiong, Xuya ^[1]; ^[3]; Li, Yaping ^[1]; Kuang, Yun ^[1]; Sun, Xiaoming ^[4]

Beijing Univ. of Chemical Technology, Beijing (China). State Key Lab. of Chemical Resource Engineering
Beijing Univ. of Chemical Technology, Beijing (China). State Key Lab. of Chemical Resource Engineering; Yale Univ., West Haven, CT (United States). Dept. of Chemistry and Energy Sciences Inst.
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Beijing Univ. of Chemical Technology, Beijing (China). State Key Lab. of Chemical Resource Engineering; Beijing Univ. of Chemical Technology, Beijing (China). College of Energy, Beijing Advanced Innovation Center for Soft Matter Science and Engineering

Atomic composition tuning and defect engineering are effective strategies to enhance the catalytic performance of multicomponent catalysts by improving the synergetic effect; however, it remains challenging to dramatically tune the active sites on multicomponent materials through simultaneous defect engineering at the atomic scale because of the similarities of the local environment. Here in this paper, using the oxygen evolution reaction (OER) as a probe reaction, we deliberately introduced 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 dramatically enhanced 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 evolution process. This defect engineering strategy provides new insights into catalysts at the atomic scale and should be beneficial for the design of a variety of catalysts.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: SC0012704

OSTI ID:: 1473662

Alternate ID(s):: OSTI ID: 22858213

Report Number(s):: BNL--209054-2018-JAAM

Journal Information:: Nano Research, Journal Name: Nano Research Journal Issue: 9 Vol. 11; ISSN 1998-0124

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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