FeN4 Sites Embedded into Carbon Nanofiber Integrated with Electrochemically Exfoliated Graphene for Oxygen Evolution in Acidic Medium

被引:230
作者
Lei, Chaojun [1 ]
Chen, Hengquan [2 ]
Cao, Junhui [1 ]
Yang, Jian [1 ]
Qiu, Ming [3 ]
Xia, Ying [3 ]
Yuan, Chris [4 ]
Yang, Bin [1 ]
Li, Zhongjian [1 ]
Zhang, Xingwang [1 ]
Lei, Lecheng [1 ]
Abbott, Janel [5 ]
Zhong, Yu [6 ]
Xia, Xinhui [6 ]
Wu, Gang [5 ]
He, Qinggang [2 ]
Hou, Yang [1 ]
机构
[1] Zhejiang Univ, Coll Chem & Biol Engn, Minist Educ, Key Lab Biomass Chem Engn, Hangzhou 310027, Zhejiang, Peoples R China
[2] Zhejiang Univ, Coll Chem & Biol Engn, Zhejiang Prov Key Lab Adv Chem Engn Manufacture T, Hangzhou 310027, Zhejiang, Peoples R China
[3] Cent China Normal Univ, Coll Phys Sci & Technol, Inst Nanosci & Nanotechnol, Wuhan 430079, Hubei, Peoples R China
[4] Case Western Reserve Univ, Dept Mech & Aerosp Engn, 10900 Euclid Ave, Cleveland, OH 44106 USA
[5] Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
[6] Zhejiang Univ, Sch Mat Sci & Engn, Key Lab Adv Mat & Applicat Batteries Zhejiang Pro, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China
关键词
acidic electrolyte; electrocatalysis; Fe-N-4; sites; nanocarbon; water oxidation; WATER OXIDATION; ACTIVE-SITES; ELECTROCATALYST; CATALYST; NANOPARTICLES; DESIGN;
D O I
10.1002/aenm.201801912
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Development of inexpensive and efficient oxygen evolution reaction (OER) catalysts in acidic environment is very challenging, but it is important for practical proton exchange membrane water electrolyzers. A molecular iron-nitrogen coordinated carbon nanofiber is developed, which is supported on an electrochemically exfoliated graphene (FeN4/NF/EG) electrocatalyst through carbonizing the precursor composed of iron ions absorbed on polyaniline-electrodeposited EG. Benefitting from the unique 3D structure, the FeN4/NF/EG hybrid exhibits a low overpotential of approximate to 294 mV at 10 mA cm(-2) for the OER in acidic electrolyte, which is much lower than that of commercial Ir/C catalysts (320 mV) as well as all previously reported acid transitional metal-derived OER electrocatalysts. X-ray absorption spectroscopy coupled with a designed poisoning experiment reveals that the molecular Fe-N-4 species are identified as active centers for the OER in acid. The first-principles-based calculations verify that the Fe-N-4-doped carbon structure is capable of reducing the potential barriers and boosting the electrocatalytic OER activity in acid.
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页数:7
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