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Title: Structure-property relationship of graphene coupled metal (Ni, Co, Fe) (oxy)hydroxides for efficient electrochemical evolution of oxygen

Abstract

Design of high-efficiency electrocatalysts for the oxygen evolution reaction (OER) is critical to meet future energy demands. A series of heterogeneous electrocatalysts based on graphene coupled mixed-metal (oxy)hydroxides containing specific concentrations of nickel, cobalt, and iron were synthesized to investigate the influence of metal composition on the structure, properties, and activities for OER. The addition of iron led to isolated metal (oxy)hydroxide sheets from a few hundred nanometers to less than 5 nm, leading to a high surface area. The increased d-spacing between layers of hydroxide and abundant hydroxyl groups adsorbed on the surface of the electrocatalysts contribute to better catalytic performance as displayed by the remarkable improvement in Tafel slopes. In addition, the presence of cobalt and nickel can aid in lowering the onset potential of OER. Small amounts of iron in NiFe and NiCoFe systems were found to significantly decrease the overpotential. The best OER electrocatalysts of the series were obtained for the ternary metal hydroxide of composition Ni0.33Co0.34Fe0.33, which generates a low overpotential of 0.332 V in reaching 10 mA cm-1 in 0.1 M KOH and the Tafel slope is as low as 51 mV dec-1. Density functional theory calculations demonstrate the improvements of electronic structure andmore » free energy changes of the ternary metal oxyhydroxide for more efficient OER electrocatalysis. Altogether, this work provides a solid foundation for further development of high-efficiency, scalable, and cost-effective mixed-metal (oxy)hydroxide electrocatalysts.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Henan Univ., Kaifeng (China)
Publication Date:
Research Org.:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1598210
Alternate Identifier(s):
OSTI ID: 1558708
Grant/Contract Number:  
FG02-86ER13622
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 377; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; water electrolysis; metal (oxy)hydroxide; graphene; oxygen evolution reaction; density functional theory (DFT)

Citation Formats

He, Junkai, Wu, Tianli, Chen, Sheng-Yu, Miao, Ran, Dang, Yanliu, Zhong, Wei, Wang, Mingchao, Jiang, Ting, and Suib, Steven L. Structure-property relationship of graphene coupled metal (Ni, Co, Fe) (oxy)hydroxides for efficient electrochemical evolution of oxygen. United States: N. p., 2019. Web. doi:10.1016/j.jcat.2019.08.006.
He, Junkai, Wu, Tianli, Chen, Sheng-Yu, Miao, Ran, Dang, Yanliu, Zhong, Wei, Wang, Mingchao, Jiang, Ting, & Suib, Steven L. Structure-property relationship of graphene coupled metal (Ni, Co, Fe) (oxy)hydroxides for efficient electrochemical evolution of oxygen. United States. https://doi.org/10.1016/j.jcat.2019.08.006
He, Junkai, Wu, Tianli, Chen, Sheng-Yu, Miao, Ran, Dang, Yanliu, Zhong, Wei, Wang, Mingchao, Jiang, Ting, and Suib, Steven L. Fri . "Structure-property relationship of graphene coupled metal (Ni, Co, Fe) (oxy)hydroxides for efficient electrochemical evolution of oxygen". United States. https://doi.org/10.1016/j.jcat.2019.08.006. https://www.osti.gov/servlets/purl/1598210.
@article{osti_1598210,
title = {Structure-property relationship of graphene coupled metal (Ni, Co, Fe) (oxy)hydroxides for efficient electrochemical evolution of oxygen},
author = {He, Junkai and Wu, Tianli and Chen, Sheng-Yu and Miao, Ran and Dang, Yanliu and Zhong, Wei and Wang, Mingchao and Jiang, Ting and Suib, Steven L.},
abstractNote = {Design of high-efficiency electrocatalysts for the oxygen evolution reaction (OER) is critical to meet future energy demands. A series of heterogeneous electrocatalysts based on graphene coupled mixed-metal (oxy)hydroxides containing specific concentrations of nickel, cobalt, and iron were synthesized to investigate the influence of metal composition on the structure, properties, and activities for OER. The addition of iron led to isolated metal (oxy)hydroxide sheets from a few hundred nanometers to less than 5 nm, leading to a high surface area. The increased d-spacing between layers of hydroxide and abundant hydroxyl groups adsorbed on the surface of the electrocatalysts contribute to better catalytic performance as displayed by the remarkable improvement in Tafel slopes. In addition, the presence of cobalt and nickel can aid in lowering the onset potential of OER. Small amounts of iron in NiFe and NiCoFe systems were found to significantly decrease the overpotential. The best OER electrocatalysts of the series were obtained for the ternary metal hydroxide of composition Ni0.33Co0.34Fe0.33, which generates a low overpotential of 0.332 V in reaching 10 mA cm-1 in 0.1 M KOH and the Tafel slope is as low as 51 mV dec-1. Density functional theory calculations demonstrate the improvements of electronic structure and free energy changes of the ternary metal oxyhydroxide for more efficient OER electrocatalysis. Altogether, this work provides a solid foundation for further development of high-efficiency, scalable, and cost-effective mixed-metal (oxy)hydroxide electrocatalysts.},
doi = {10.1016/j.jcat.2019.08.006},
journal = {Journal of Catalysis},
number = C,
volume = 377,
place = {United States},
year = {Fri Aug 23 00:00:00 EDT 2019},
month = {Fri Aug 23 00:00:00 EDT 2019}
}

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