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Title: Rational Design and Synthesis of Hierarchical Porous Mn–N–C Nanoparticles with Atomically Dispersed MnNx Moieties for Highly Efficient Oxygen Reduction Reaction

Abstract

Developing transition-metal excluding iron and cobalt–nitrogen–carbon (M–N–C) electrocatalysts for the oxygen reduction reaction (ORR) is critical to substantially promote the development of precious-metal-free metal–air batteries and fuel cells. In the work, Mn–N–C nanoparticles with atomically dispersed MnNx moieties were synthesized by pyrolyzing Mn-ion–dual-pyridine coordinated complex, which was obtained via a simple condensation reaction between 2,6-diamino-pyridine and 2,6-diacetyl-pyridine with MnCl 2 as the Mn source. The precursor features with a characteristic structure of dual-pyridine ligand, which possesses a strong coordinating capability for Mn 2+, facilitating the formation of highly dispersed nitrogen-coordinated Mn sites (MnN x). Attributed to the highly active atomic MnN x sites, hierarchical pore structure, and high surface area of the Mn–N–C derived from the new precursor, it exhibits outstanding ORR performance in 0.1 M KOH with an almost direct four-electron reaction path and high selectivity of O 2 into H 2O (low H2O2 production <3.5%). The half-wave potential of Mn–N–C is 0.88 V vs RHE, which is 20 mV higher than that of commercial Pt/C catalyst and reaches to the level of Fe–N–C catalyst obtained by the same method. Meanwhile, the feasibility of Mn–N–C for practical application is validated by its higher-performance power output in Zn–air battery withmore » a maximum power density of 132 mW cm –2 compared to that of Pt/C (121 mW cm –2) using the same catalyst loading of 1.0 mg cm –2. This work develops a convenient route to develop non-Fe or Co–N–C electrocatalyst for the ORR.« less

Authors:
 [1];  [1];  [2];  [1];  [3];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]
  1. Guangxi Univ., Nanning (China). Collaborative Innovation Center of Sustainable Energy Materials; Ministry of Education, Nanning (China). Guangxi Key Lab. of Electrochemical Energy Materials, Key Lab. of New processing Technology for Non-ferrous Metal and Materials
  2. Inst. of Chemical and Engineering Sciences, Jurong Island (Singapore)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key R&D Plan of China; National Natural Science Foundation of China (NNSFC); Innovation Project of Guangxi Graduate Education of China
OSTI Identifier:
1656593
Report Number(s):
BNL-216322-2020-JAAM
Journal ID: ISSN 2168-0485
Grant/Contract Number:  
SC0012704; 2017YFB0103001; U1705252; AB16380030; AA17204083; YCBZ2020011
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Sustainable Chemistry & Engineering
Additional Journal Information:
Journal Volume: 8; Journal Issue: 25; Journal ID: ISSN 2168-0485
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Mn-N-C; MnNx moieties; oxygen reduction reaction; fuel cells; Zn-air batteries

Citation Formats

Wang, Yunqiu, Zhang, Xiaoran, Xi, Shibo, Xiang, Xue, Du, Yonghua, Chen, Pinsong, Lyu, Dandan, Wang, Shuangbao, Tian, Zhi Qun, and Shen, Pei Kang. Rational Design and Synthesis of Hierarchical Porous Mn–N–C Nanoparticles with Atomically Dispersed MnNx Moieties for Highly Efficient Oxygen Reduction Reaction. United States: N. p., 2020. Web. doi:10.1021/acssuschemeng.0c01882.
Wang, Yunqiu, Zhang, Xiaoran, Xi, Shibo, Xiang, Xue, Du, Yonghua, Chen, Pinsong, Lyu, Dandan, Wang, Shuangbao, Tian, Zhi Qun, & Shen, Pei Kang. Rational Design and Synthesis of Hierarchical Porous Mn–N–C Nanoparticles with Atomically Dispersed MnNx Moieties for Highly Efficient Oxygen Reduction Reaction. United States. doi:10.1021/acssuschemeng.0c01882.
Wang, Yunqiu, Zhang, Xiaoran, Xi, Shibo, Xiang, Xue, Du, Yonghua, Chen, Pinsong, Lyu, Dandan, Wang, Shuangbao, Tian, Zhi Qun, and Shen, Pei Kang. Fri . "Rational Design and Synthesis of Hierarchical Porous Mn–N–C Nanoparticles with Atomically Dispersed MnNx Moieties for Highly Efficient Oxygen Reduction Reaction". United States. doi:10.1021/acssuschemeng.0c01882.
@article{osti_1656593,
title = {Rational Design and Synthesis of Hierarchical Porous Mn–N–C Nanoparticles with Atomically Dispersed MnNx Moieties for Highly Efficient Oxygen Reduction Reaction},
author = {Wang, Yunqiu and Zhang, Xiaoran and Xi, Shibo and Xiang, Xue and Du, Yonghua and Chen, Pinsong and Lyu, Dandan and Wang, Shuangbao and Tian, Zhi Qun and Shen, Pei Kang},
abstractNote = {Developing transition-metal excluding iron and cobalt–nitrogen–carbon (M–N–C) electrocatalysts for the oxygen reduction reaction (ORR) is critical to substantially promote the development of precious-metal-free metal–air batteries and fuel cells. In the work, Mn–N–C nanoparticles with atomically dispersed MnNx moieties were synthesized by pyrolyzing Mn-ion–dual-pyridine coordinated complex, which was obtained via a simple condensation reaction between 2,6-diamino-pyridine and 2,6-diacetyl-pyridine with MnCl2 as the Mn source. The precursor features with a characteristic structure of dual-pyridine ligand, which possesses a strong coordinating capability for Mn2+, facilitating the formation of highly dispersed nitrogen-coordinated Mn sites (MnNx). Attributed to the highly active atomic MnNx sites, hierarchical pore structure, and high surface area of the Mn–N–C derived from the new precursor, it exhibits outstanding ORR performance in 0.1 M KOH with an almost direct four-electron reaction path and high selectivity of O2 into H2O (low H2O2 production <3.5%). The half-wave potential of Mn–N–C is 0.88 V vs RHE, which is 20 mV higher than that of commercial Pt/C catalyst and reaches to the level of Fe–N–C catalyst obtained by the same method. Meanwhile, the feasibility of Mn–N–C for practical application is validated by its higher-performance power output in Zn–air battery with a maximum power density of 132 mW cm–2 compared to that of Pt/C (121 mW cm–2) using the same catalyst loading of 1.0 mg cm–2. This work develops a convenient route to develop non-Fe or Co–N–C electrocatalyst for the ORR.},
doi = {10.1021/acssuschemeng.0c01882},
journal = {ACS Sustainable Chemistry & Engineering},
issn = {2168-0485},
number = 25,
volume = 8,
place = {United States},
year = {2020},
month = {6}
}

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