Entropy Enhanced Perovskite Oxide Ceramic for Efficient Electrochemical Reduction of Oxygen to Hydrogen Peroxide

被引:74
作者
Chen, Ziliang [1 ,2 ]
Wu, Jie [1 ]
Chen, Zhengran [3 ]
Yang, Hongyuan [2 ]
Zou, Kai [3 ]
Zhao, Xiangyong [5 ]
Liang, Ruihong [3 ]
Dong, Xianlin [3 ]
Menezes, Prashanth W. [2 ,4 ]
Kang, Zhenhui [1 ]
机构
[1] Soochow Univ, Joint Int Res Lab Carbon Based Funct Mat & Device, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Inst Funct Nano & Soft Mat FUNSOM, Suzhou 215123, Peoples R China
[2] Tech Univ Berlin, Dept Chem Metalorgan & Inorgan Mat, Str 17 Juni 135,Sekr C2, D-10623 Berlin, Germany
[3] Chinese Acad Sci, Shanghai Inst Ceram, Key Lab Inorgan Funct Mat & Devices, 588 Heshuo Rd, Shanghai 201800, Peoples R China
[4] Helmholtz Zentrum Berlin Mat & Energie, Mat Chem Grp Thin Film Catalysis CatLab, Albert Einstein Str 15, D-12489 Berlin, Germany
[5] Shanghai Normal Univ, Dept Phys, Key Lab Optoelect Mat & Device, Shanghai 200234, Peoples R China
基金
国家重点研发计划;
关键词
Electrocatalysis; High Entropy; Hydrogen Peroxide; Oxygen Reduction Reaction; Perovskite Oxide Ceramic; INTERFACE ELECTRON-TRANSFER; EVOLUTION; VACANCIES; CATALYST; CARBIDE;
D O I
10.1002/anie.202200086
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The electrochemical oxygen reduction reaction (ORR) offers a most promising and efficient route to produce hydrogen peroxide (H2O2), yet the lack of cost-effective and high-performance electrocatalysts have restricted its practical application. Herein, an entropy-enhancement strategy has been employed to enable the low-cost perovskite oxide to effectively catalyze the electrosynthesis of H2O2. The optimized Pb(NiWMnNbZrTi)(1/6)O-3 ceramic is available on a kilogram-scale and displays commendable ORR activity in alkaline media with high selectivity over 91 % across the wide potential range for H2O2 including an outstanding degradation property for organic dyes through the Fenton process. The exceptional performance of this perovskite oxide is attributed to the entropy stabilization-induced polymorphic transformation assuring the robust structural stability, decreased charge mobility as well as synergistic catalytic effects which we confirm using advanced in situ Raman, transient photovoltage, Rietveld refinement as well as finite elemental analysis.
引用
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页数:10
相关论文
共 61 条
[1]  
[Anonymous], 2014, ANGEW CHEM, V126, P4670
[2]   Carbon-supported MnO2 nanoflowers: Introducing oxygen vacancies for optimized volcano-type electrocatalytic activities towards H2O2 generation [J].
Aveiro, Luci R. ;
da Silva, Anderson G. M. ;
Antonin, Vanessa S. ;
Candido, Eduardo G. ;
Parreira, Luanna S. ;
Geonmonond, Rafael S. ;
de Freitas, Isabel C. ;
Lanza, Marcos R. V. ;
Camargo, Pedro H. C. ;
Santos, Mauro C. .
ELECTROCHIMICA ACTA, 2018, 268 :101-110
[3]   Tuning electrochemially driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis [J].
Baeumer, Christoph ;
Li, Jiang ;
Lu, Qiyang ;
Liang, Allen Yu-Lun ;
Jin, Lei ;
Martins, Henrique Perin ;
Duchon, Tomas ;
GloEss, Maria ;
Gericke, Sabrina M. ;
Wohlgemuth, Marcus A. ;
Giesen, Margret ;
Penn, Emily E. ;
Dittmann, Regina ;
Gunkel, Felix ;
Waser, Rainer ;
Bajdich, Michal ;
Nemsak, Slavomir ;
Mefford, J. Tyler ;
Chueh, William C. .
NATURE MATERIALS, 2021, 20 (05) :674-+
[4]   High-Entropy Alloys as a Discovery Platform for Electrocatalysis [J].
Batchelor, Thomas A. A. ;
Pedersen, Jack K. ;
Winther, Simon H. ;
Castelli, Ivano E. ;
Jacobsen, Karsten W. ;
Rossmeisl, Jan .
JOULE, 2019, 3 (03) :834-845
[5]   Doping strain induced bi-Ti3+ pairs for efficient N2 activation and electrocatalytic fixation [J].
Cao, Na ;
Chen, Zheng ;
Zang, Ketao ;
Xu, Jie ;
Zhong, Jun ;
Luo, Jun ;
Xu, Xin ;
Zheng, Gengfeng .
NATURE COMMUNICATIONS, 2019, 10 (1)
[6]   Zirconia on Reduced Graphene Oxide Sheets: Synergistic Catalyst with High Selectivity for H2O2 Electrogeneration [J].
Carneiro, Jussara F. ;
Paulo, Maria J. ;
Siaj, Mohamed ;
Tavares, Ana C. ;
Lanza, Marcos R. V. .
CHEMELECTROCHEM, 2017, 4 (03) :508-513
[7]   An Amorphous Nickel-Iron-Based Electrocatalyst with Unusual Local Structures for Ultrafast Oxygen Evolution Reaction [J].
Chen, Gao ;
Zhu, Yapping ;
Chen, Hao Ming ;
Hu, Zhiwei ;
Hung, Sung-Fu ;
Ma, Nana ;
Dai, Jie ;
Lin, Hong-Ji ;
Chen, Chien-Te ;
Zhou, Wei ;
Shao, Zongping .
ADVANCED MATERIALS, 2019, 31 (28)
[8]   Highly Selective Carbon Dioxide Electroreduction on Structure-Evolved Copper Perovskite Oxide toward Methane Production [J].
Chen, Shenghua ;
Su, Yaqiong ;
Deng, Peilin ;
Qi, Ruijuan ;
Zhu, Jiexin ;
Chen, Jinxi ;
Wang, Zhitong ;
Zhou, Liang ;
Guo, Xingpeng ;
Xia, Bao Yu .
ACS CATALYSIS, 2020, 10 (08) :4640-4646
[9]  
Chen Z., ANGEW CHEM INT EDIT, V2022
[10]   Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution [J].
Dai, Jie ;
Zhu, Yinlong ;
Tahini, Hassan A. ;
Lin, Qian ;
Chen, Yu ;
Guan, Daqin ;
Zhou, Chuan ;
Hu, Zhiwei ;
Lin, Hong-Ji ;
Chan, Ting-Shan ;
Chen, Chien-Te ;
Smith, Sean C. ;
Wang, Huanting ;
Zhou, Wei ;
Shao, Zongping .
NATURE COMMUNICATIONS, 2020, 11 (01)