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

被引:67
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
收藏
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
    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.
    [J]. ELECTROCHIMICA ACTA, 2018, 268 : 101 - 110
  • [3] Tuning electrochemially driven surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis
    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.
    [J]. NATURE MATERIALS, 2021, 20 (05) : 674 - +
  • [4] High-Entropy Alloys as a Discovery Platform for Electrocatalysis
    Batchelor, Thomas A. A.
    Pedersen, Jack K.
    Winther, Simon H.
    Castelli, Ivano E.
    Jacobsen, Karsten W.
    Rossmeisl, Jan
    [J]. JOULE, 2019, 3 (03) : 834 - 845
  • [5] Doping strain induced bi-Ti3+ pairs for efficient N2 activation and electrocatalytic fixation
    Cao, Na
    Chen, Zheng
    Zang, Ketao
    Xu, Jie
    Zhong, Jun
    Luo, Jun
    Xu, Xin
    Zheng, Gengfeng
    [J]. NATURE COMMUNICATIONS, 2019, 10 (1)
  • [6] Zirconia on Reduced Graphene Oxide Sheets: Synergistic Catalyst with High Selectivity for H2O2 Electrogeneration
    Carneiro, Jussara F.
    Paulo, Maria J.
    Siaj, Mohamed
    Tavares, Ana C.
    Lanza, Marcos R. V.
    [J]. CHEMELECTROCHEM, 2017, 4 (03): : 508 - 513
  • [7] An Amorphous Nickel-Iron-Based Electrocatalyst with Unusual Local Structures for Ultrafast Oxygen Evolution Reaction
    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
    [J]. ADVANCED MATERIALS, 2019, 31 (28)
  • [8] Highly Selective Carbon Dioxide Electroreduction on Structure-Evolved Copper Perovskite Oxide toward Methane Production
    Chen, Shenghua
    Su, Yaqiong
    Deng, Peilin
    Qi, Ruijuan
    Zhu, Jiexin
    Chen, Jinxi
    Wang, Zhitong
    Zhou, Liang
    Guo, Xingpeng
    Xia, Bao Yu
    [J]. 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
    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
    [J]. NATURE COMMUNICATIONS, 2020, 11 (01)