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

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

doi:10.1002/anie.201804881

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

Journal Article · 10 June 2018 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.201804881 · OSTI ID:1454823

Cai, Zhao ^[1]; Zhou, Daojin ^[2]; Wang, Maoyu ^[3];

^[4]; Wu, Yueshen ^[5]; Wu, Zishan ^[5]; Tian, Yang ^[2]; Xiong, Xuya ^[2]; Li, Yaping ^[2]; Liu, Wen ^[1]; Siahrostami, Samira ^[6]; Kuang, Yun ^[2]; Yang, Xiao -Qing ^[4]; Duan, Haohong ^[7]; Feng, Zhenxing ^[3]; Wang, Hailiang ^[5]; Sun, Xiaoming ^[2]

Beijing Univ. of Chemical Technology, Beijing (China); Yale Univ., New Haven, CT (United States)
Beijing Univ. of Chemical Technology, Beijing (China)
Oregon State Univ., Corvallis, OR (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Yale Univ., New Haven, CT (United States)
Stanford Univ., Stanford, CA (United States)
Univ. of Oxford, Oxford (United Kingdom)

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. Here 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/cm², which is among the best OER catalytic performance reported 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. Lastly, these results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.

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

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1454823

Report Number(s):: BNL-205757-2018-JAAM

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 30 Vol. 57; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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