The strain induced synergistic catalysis of FeN4 and MnN3 dual-site catalysts for oxygen reduction in proton-/anion- exchange membrane fuel cells

被引：115

作者：

Huang, Shiqing ^{[1
]}

Qiao, Zelong ^{[1
]}

Sun, Panpan ^{[1
]}

Qiao, Kangwei ^{[1
]}

Pei, Kun ^{[1
]}

Yang, Liu ^{[1
]}

Xu, Haoxiang ^{[1
]}

Wang, Shitao ^{[1
]}

Huang, Yan ^{[1
]}

Yan, Yushan ^{[2
]}

Cao, Dapeng ^{[1
]}

机构：

[1] Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China

[2] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 317卷

关键词：

Dual-atom catalysts; Oxygen reduction reaction; Strain effect; Synergistic catalysis; Proton-/anion-exchange membrane fuel cells; ELECTROCATALYSTS; SUPERFAMILY;

D O I：

10.1016/j.apcatb.2022.121770

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 Fe-N-C single-atom catalysts (SACs) have been widely explored for oxygen reduction reaction (ORR) in fuel cells. However, how to improve the ORR activity by tailoring the electronic structure of Fe-N-C catalysts is challenging. Herein, we synthesize a Fe-Mn-N-C dual-atom catalyst (DAC) with new local structure of FeN4-MnN3 moiety, and it exhibits ultralow H2O2 yield and better ORR performance than Fe-N-C and Mn-N-C SACs. Importantly, the Fe-Mn-N-C-based proton -/anion-exchange membrane fuel cells present ultrahigh power densities of 1.048 W cm(-2) and 1.321 W cm(-2), respectively. DFT results reveal that the strain yielded by the formation of Mn-Fe bond significantly optimizes the electronic structure of the Fe-Mn-N-C, and the co-adsorption of the Fe-Mn dual-sites for *OOH not only almost completely suppresses the 2e-ORR, but also breaks the linear correlation between GOH* and GOOH* proposed by Norskov et al., which provides a new route for the design of dual-site catalysts.

引用

页数：9

共 56 条

[1] High-performing commercial Fe-N-C cathode electrocatalyst for anion-exchange membrane fuel cells [J].

Adabi, Horie ;

Shakouri, Abolfazl ;

Ul Hassan, Noor ;

Varcoe, John R. ;

Zulevi, Barr ;

Serov, Alexey ;

Regalbuto, John R. ;

Mustain, William E. .

NATURE ENERGY, 2021, 6 (08) :834-843

[2] Historical development and novel concepts on electrolytes for aqueous rechargeable batteries [J].

Chen, Shigang ;

Zhang, Mengfei ;

Zou, Peimiao ;

Sun, Boyao ;

Tao, Shanwen .

ENERGY & ENVIRONMENTAL SCIENCE, 2022, 15 (05) :1805-1839

[3] Enhanced performance of atomically dispersed dual-site Fe-Mn electrocatalysts through cascade reaction mechanism [J].

Chen, Zhe ;

Liao, Xiaobin ;

Sun, Congli ;

Zhao, Kangning ;

Ye, Daixin ;

Li, Jiantao ;

Wu, Gang ;

Fang, Jianhui ;

Zhao, Hongbin ;

Zhang, Jiujun .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 288

[4] Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe-N-C Catalysts [J].

Choi, Chang Hyuck ;

Choi, Won Seok ;

Kasian, Olga ;

Mechler, Anna K. ;

Sougrati, Moulay Tahar ;

Bruller, Sebastian ;

Strickland, Kara ;

Jia, Qingying ;

Mukerjee, Sanjeev ;

Mayrhofer, Karl J. J. ;

Jaouen, Frederic .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (30) :8809-8812

[5] Opportunities and challenges for a sustainable energy future [J].

Chu, Steven ;

Majumdar, Arun .

NATURE, 2012, 488 (7411) :294-303

[6] Crystal Orbital Hamilton Population (COHP) Analysis As Projected from Plane-Wave Basis Sets [J].

Deringer, Volker L. ;

Tchougreeff, Andrei L. ;

Dronskowski, Richard .

JOURNAL OF PHYSICAL CHEMISTRY A, 2011, 115 (21) :5461-5466

[7] General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities [J].

Fei, Huilong ;

Dong, Juncai ;

Feng, Yexin ;

Allen, Christopher S. ;

Wan, Chengzhang ;

Volosskiy, Boris ;

Li, Mufan ;

Zhao, Zipeng ;

Wang, Yiliu ;

Sun, Hongtao ;

An, Pengfei ;

Chen, Wenxing ;

Guo, Zhiying ;

Lee, Chain ;

Chen, Dongliang ;

Shakir, Imran ;

Liu, Mingjie ;

Hu, Tiandou ;

Li, Yadong ;

Kirkland, Angus I. ;

Duan, Xiangfeng ;

Huang, Yu .

NATURE CATALYSIS, 2018, 1 (01) :63-72

[8] Stability of iron species in heat-treated polyaniline-iron-carbon polymer electrolyte fuel cell cathode catalysts [J].

Ferrandon, Magali ;

Wang, Xiaoping ;

Kropf, A. Jeremy ;

Myers, Deborah J. ;

Wu, Gang ;

Johnston, Christina M. ;

Zelenay, Piotr .

ELECTROCHIMICA ACTA, 2013, 110 :282-291

[9] Degradation by Hydrogen Peroxide of Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction [J].

Goellner, Vincent ;

Armel, Vanessa ;

Zitolo, Andrea ;

Fonda, Emiliano ;

Jaouen, Frederic .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2015, 162 (06) :H403-H414

[10] Designing highly efficient dual-metal single-atom electrocatalysts for the oxygen reduction reaction inspired by biological enzyme systems [J].

Gong, Shipeng ;

Wang, Changlai ;

Jiang, Peng ;

Hu, Lin ;

Lei, Hu ;

Chen, Qianwang .

JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (27) :13254-13262

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