Development of novel and robust oxygen evolution reaction (OER) catalysts with well-modulated atomic and electronic structure remains a challenge. Compared to the well-known metal hydroxides or (oxyhydr)oxides with lamellar structure, delafossites (ABO(2)) are characterized by alternating layers of A cations and edge-sharing BO2 octahedra, but are rarely used in OER due to their poor electron conductivity and intrinsic activity. Here, we propose a delafossite analog by mutation of metal oxyhydroxide and delafossite based on first-principles calculations. Modulation on the electronic structure due to distortion of the original crystal field of the BO2 layers is calculated to enhance electron conductivity and catalytic activity. Inspired by the theoretical design, we have experimentally realized the delafossite analog by electrochemical self-reconstruction (ECSR). Operando X-ray absorption spectroscopy and other experimental techniques reveal the formation of delafossite analog with Ag intercalated into bimetallic cobalt-iron (oxyhydr) oxide layers from a metastable precursor through amorphization. Benefirting from the featured local electronic and geometric structures, the delafossite analog shows superior OER activity, affording a current density of 10 mA.cm(-2) at an overpotential of 187 mV and an excellent stability (300 h) in alkaline conditions.
机构:
Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United StatesDepartment of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
Lutterman, Daniel A.
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Surendranath, Yogesh
Nocera, Daniel G.
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Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United StatesDepartment of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
Nocera, Daniel G.
Journal of the American Chemical Society,
2009,
131
(11):
: 3838
-
3839
机构:
Zhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Zhang, Xiaojian
Feng, Chao
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Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Feng, Chao
Fan, Zeyu
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Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Fan, Zeyu
Zhang, Beibei
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Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Zhang, Beibei
Xiao, Yequan
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Xiangtan Univ, Sch Phys & Optoelect, Xiangtan 411105, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Xiao, Yequan
Mavric, Andraz
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Univ Nova Gorica, Mat Res Lab, Vipavska 13, SI-5000 Nova Gorica, SloveniaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Mavric, Andraz
Pastukhova, Nadiia
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Univ Nova Gorica, Mat Res Lab, Vipavska 13, SI-5000 Nova Gorica, SloveniaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Pastukhova, Nadiia
Valant, Matjaz
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Univ Nova Gorica, Mat Res Lab, Vipavska 13, SI-5000 Nova Gorica, SloveniaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Valant, Matjaz
Han, Yi-Fan
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Zhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
Han, Yi-Fan
Li, Yanbo
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Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Peoples R ChinaZhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China
机构:
Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Zhao, Fuzhen
Mao, Xinyu
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Mao, Xinyu
Zheng, Xin
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China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Zheng, Xin
Liu, Huicong
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Liu, Huicong
Zhu, Liqun
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Zhu, Liqun
Li, Weiping
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Li, Weiping
Wang, Ze
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
Wang, Ze
Chen, Haining
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Beihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R ChinaBeihang Univ, Sch Mat Sci & Engn, 37 Xueyuan Rd, Beijing 100191, Peoples R China
机构:
Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China
Zhao, Qiang
Liu, Lin
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Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China
Liu, Lin
Li, Dandan
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Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China
Li, Dandan
Zhong, Dazhong
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Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China
Zhong, Dazhong
Hao, Genyan
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Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China
Hao, Genyan
Li, Jinping
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Taiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R ChinaTaiyuan Univ Technol, Res Inst Special Chem, Taiyuan 030024, Shanxi, Peoples R China