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Title: Introducing Fe 2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity

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 Ni 2+ with Fe 2+ to introduce Fe–O–Fe moieties. These Fe 2+–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 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.
Authors:
 [1] ;  [2] ;  [3] ; ORCiD logo [4] ;  [5] ;  [5] ;  [2] ;  [2] ;  [2] ;  [1] ;  [6] ;  [2] ;  [4] ;  [7] ;  [3] ;  [5] ;  [2]
  1. Beijing Univ. of Chemical Technology, Beijing (China); Yale Univ., New Haven, CT (United States)
  2. Beijing Univ. of Chemical Technology, Beijing (China)
  3. Oregon State Univ., Corvallis, OR (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Yale Univ., New Haven, CT (United States)
  6. Stanford Univ., Stanford, CA (United States)
  7. Univ. of Oxford, Oxford (United Kingdom)
Publication Date:
Report Number(s):
BNL-205757-2018-JAAM
Journal ID: ISSN 1433-7851
Grant/Contract Number:
SC0012704; DESC0012704; No.DEAC02-06CH11357.
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1454823
Alternate Identifier(s):
OSTI ID: 1457470

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, and Sun, Xiaoming. Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity. United States: N. p., Web. doi:10.1002/anie.201804881.
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. Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity. United States. doi:10.1002/anie.201804881.
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, and Sun, Xiaoming. 2018. "Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity". United States. doi:10.1002/anie.201804881.
@article{osti_1454823,
title = {Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity},
author = {Cai, Zhao and Zhou, Daojin and Wang, Maoyu and Bak, Seongmin and Wu, Yueshen and Wu, Zishan and Tian, Yang and Xiong, Xuya and Li, Yaping and Liu, Wen and Siahrostami, Samira and Kuang, Yun and Yang, Xiao -Qing and Duan, Haohong and Feng, Zhenxing and Wang, Hailiang and Sun, Xiaoming},
abstractNote = {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.},
doi = {10.1002/anie.201804881},
journal = {Angewandte Chemie (International Edition)},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {6}
}