Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity

Zhao Cai; Daojin Zhou; Maoyu Wang; Seong-Min Bak; Yueshen Wu; Zishan Wu; Yang Tian; Xuya Xiong; Yaping Li; Wen Liu; Samira Siahrostami; Yun Kuang; Xiao-Qing Yang; Haohong Duan; Zhenxing Feng; Hailiang Wang; Xiaoming Sun

doi:10.1002/anie.201804881

Introducing Fe²⁺ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity

Angew Chem Int Ed Engl. 2018 Jul 20;57(30):9392-9396. doi: 10.1002/anie.201804881. Epub 2018 Jun 27.

Authors

Zhao Cai^{1

2}, Daojin Zhou¹, Maoyu Wang³, Seong-Min Bak⁴, Yueshen Wu², Zishan Wu², Yang Tian¹, Xuya Xiong¹, Yaping Li¹, Wen Liu^{1

2}, Samira Siahrostami⁵, Yun Kuang¹, Xiao-Qing Yang⁴, Haohong Duan⁶, Zhenxing Feng³, Hailiang Wang², Xiaoming Sun^{1

7}

Affiliations

¹ State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
² Department of Chemistry and Energy Sciences Institute, Yale University, West Haven, CT, 06516, USA.
³ School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, OR, 97331, USA.
⁴ Chemistry Division, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁵ SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, 94305, USA.
⁶ Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford, OX1 3TA, UK.
⁷ College of Energy, Beijing University of Chemical Technology, Beijing, 100029, China.

PMID: 29889350
DOI: 10.1002/anie.201804881

Abstract

Exploring materials with regulated local structures and understanding how the atomic motifs govern the reactivity and durability of catalysts are a critical challenge for designing advanced catalysts. Herein we report the tuning of the local atomic structure of nickel-iron layered double hydroxides (NiFe-LDHs) by partially substituting Ni²⁺ with Fe²⁺ to introduce Fe-O-Fe moieties. These Fe²⁺ -containing NiFe-LDHs exhibit enhanced oxygen evolution reaction (OER) activity with an ultralow overpotential of 195 mV at the current density of 10 mA cm^-2 , which is among the best OER catalytic performance to date. In-situ X-ray absorption, Raman, and electrochemical analysis jointly reveal that the Fe-O-Fe motifs could stabilize high-valent metal sites at low overpotentials, thereby enhancing the OER activity. These results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.

Keywords: NiFe catalyst; iron; layered double hydroxides; local structure; oxygen evolution reaction (OER).