Highly Efficient Oxygen Evolution by a Thermocatalytic Process Cascaded Electrocatalysis Over Sulfur-Treated Fe-Based Metal-Organic-Frameworks

被引:95
作者
Feng, Kun [1 ]
Zhang, Duo [2 ]
Liu, Fangfang [1 ]
Li, Hui [2 ]
Xu, Jiabin [1 ]
Xia, Yujian [1 ]
Li, Youyong [1 ]
Lin, Haiping [1 ]
Wang, Shuao [2 ]
Shao, Mingwang [1 ]
Kang, Zhenhui [1 ]
Zhong, Jun [1 ]
机构
[1] Soochow Univ, Inst Funct Nano & Soft Mat Lab FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Peoples R China
[2] Soochow Univ, Sch Radiat Med & Protect, State Key Lab Radiat Med & Protect, Suzhou 215123, Peoples R China
基金
中国国家自然科学基金;
关键词
electrochemical OER; metal-organic-framework; sulfur-treatment; thermocatalytic processes; X-RAY-ABSORPTION; TOTAL-ENERGY CALCULATIONS; OXIDATION-STATES; CARBON; NANOSTRUCTURES; IDENTIFICATION; CATALYSTS; ARRAYS; SITES;
D O I
10.1002/aenm.202000184
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
The oxygen evolution reaction (OER) is a bottleneck process for water splitting and finding highly efficient, durable, low-cost, and earth-abundant electrocatalysts is still a major challenge. Here a sulfur-treated Fe-based metal-organic-framework is reported as a promising electrocatalyst for the OER, which shows a low overpotential of 218 mV at the current density of 10 mA cm(-2) and exhibits a very low Tafel slope of 36.2 mV dec(-1) at room temperature. It can work on high current densities of 500 and 1000 mA cm(-2) at low overpotentials of 298 and 330 mV, respectively, by keeping 97% of its initial activity after 100 h. Notably, it can achieve 1000 mA cm(-2) at 296 mV with a good stability at 50 degrees C, fully fitting the requirements for large-scale industrial water electrolysis. The high catalytic performance can be attributed to the thermocatalytic processes of H+ capture by -SO3 groups from *OH or *OOH species, which cascades to the electrocatalytic pathway and then significantly reduces the OER overpotentials.
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页数:8
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共 35 条
[1]   Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution [J].
Cao, Linlin ;
Luo, Qiquan ;
Liu, Wei ;
Lin, Yue ;
Liu, Xiaokang ;
Cao, Yuanjie ;
Zhang, Wei ;
Wu, Yuen ;
Yang, Jinlong ;
Yao, Tao ;
Wei, Shiqiang .
NATURE CATALYSIS, 2019, 2 (02) :134-141
[2]   Lattice-strained metal-organic-framework arrays for bifunctional oxygen electrocatalysis [J].
Cheng, Weiren ;
Zhao, Xu ;
Su, Hui ;
Tang, Fumin ;
Che, Wei ;
Zhang, Hui ;
Liu, Qinghua .
NATURE ENERGY, 2019, 4 (02) :115-122
[3]   Eutectic-Derived Mesoporous Ni-Fe-O Nanowire Network Catalyzing Oxygen Evolution and Overall Water Splitting [J].
Dong, Chaoqun ;
Kou, Tianyi ;
Gao, Hui ;
Peng, Zhangquan ;
Zhang, Zhonghua .
ADVANCED ENERGY MATERIALS, 2018, 8 (05)
[4]   Nickel-vanadium monolayer double hydroxide for efficient electrochemical water oxidation [J].
Fan, Ke ;
Chen, Hong ;
Ji, Yongfei ;
Huang, Hui ;
Claesson, Per Martin ;
Daniel, Quentin ;
Philippe, Bertrand ;
Rensmo, Hakan ;
Li, Fusheng ;
Luo, Yi ;
Sun, Licheng .
NATURE COMMUNICATIONS, 2016, 7
[5]   Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting [J].
Friebel, Daniel ;
Louie, Mary W. ;
Bajdich, Michal ;
Sanwald, Kai E. ;
Cai, Yun ;
Wise, Anna M. ;
Cheng, Mu-Jeng ;
Sokaras, Dimosthenis ;
Weng, Tsu-Chien ;
Alonso-Mori, Roberto ;
Davis, Ryan C. ;
Bargar, John R. ;
Norskov, Jens K. ;
Nilsson, Anders ;
Bell, Alexis T. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (03) :1305-1313
[6]   Synergism of Geometric Construction and Electronic Regulation: 3D Se-(NiCo)Sx/(OH)x Nanosheets for Highly Efficient Overall Water Splitting [J].
Hu, Congling ;
Zhang, Lei ;
Zhao, Zhi-Jian ;
Li, Ang ;
Chang, Xiaoxia ;
Gong, Jinlong .
ADVANCED MATERIALS, 2018, 30 (12)
[7]   Overall water splitting by graphdiyne-exfoliated and -sandwiched layered double-hydroxide nanosheet arrays [J].
Hui, Lan ;
Xue, Yurui ;
Huang, Bolong ;
Yu, Huidi ;
Zhang, Chao ;
Zhang, Danyan ;
Jia, Dianzeng ;
Zhao, Yingjie ;
Li, Yongjun ;
Liu, Huibiao ;
Li, Yuliang .
NATURE COMMUNICATIONS, 2018, 9
[8]   Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set [J].
Kresse, G ;
Furthmuller, J .
PHYSICAL REVIEW B, 1996, 54 (16) :11169-11186
[9]   Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set [J].
Kresse, G ;
Furthmuller, J .
COMPUTATIONAL MATERIALS SCIENCE, 1996, 6 (01) :15-50
[10]   Hydrogen-treated hematite nanostructures with low onset potential for highly efficient solar water oxidation [J].
Li, Ming ;
Deng, Jiujun ;
Pu, Aiwu ;
Zhang, Pingping ;
Zhang, Hui ;
Gao, Jing ;
Hao, Yuanyuan ;
Zhong, Jun ;
Sun, Xuhui .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (19) :6727-6733