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Title: Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MN x Active Moieties Enable Enhanced ORR Performance

Abstract

The great interest in fuel cells inspires a substantial amount of research on nonprecious metal catalysts as alternatives to Pt-based oxygen reduction reaction (ORR) electrocatalysts. In this work, bimodal template-based synthesis strategies are proposed for the scalable preparation of hierarchically porous M-N-C (M = Fe or Co) single-atom electrocatalysts featured with active and robust MN 2 active moieties. Multiscale tuning of M-N-C catalysts regarding increasing the number of active sites and boosting the intrinsic activity of each active site is realized simultaneously at a single-atom scale. In addition to the antipoisoning power and high affinity for O 2, the optimized Fe-N-C catalysts with FeN 2 active site presents a superior electrocatalytic activity for ORR with a half-wave potential of 0.927 V (vs reversible hydrogen electrode (RHE)) in an alkaline medium, which is 49 and 55 mV higher than those of the Co-N-C counterpart and commercial Pt/C, respectively. Density functional theory calculations reveal that the FeN 2 site is more active than the CoN 2 site for ORR due to the lower energy barriers of the intermediates and products involved. In conclusion, the present work may help rational design of more robust ORR electrocatalysts at the atomic level, realizing the significantmore » advances in electrochemical conversion and storage devices.« less

Authors:
 [1];  [2];  [3];  [2];  [4];  [4];  [5];  [2];  [4];  [1];  [2];  [5]; ORCiD logo [2]
  1. Washington State Univ., Pullman, WA (United States); Central China Normal Univ., Wuhan (People's Republic of China)
  2. Washington State Univ., Pullman, WA (United States)
  3. Univ. of California, Berkeley, CA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1491129
Alternate Identifier(s):
OSTI ID: 1467735; OSTI ID: 1484234
Report Number(s):
BNL-210876-2019-JAAM
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
SC0012704; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 29; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; single-atom catalysts; M-N-C catalysts; porous nanostructures; nonprecious metal catalysts; oxygen reduction reaction

Citation Formats

Zhu, Chengzhou, Shi, Qiurong, Xu, Bo Z., Fu, Shaofang, Wan, Gang, Yang, Ce, Yao, Siyu, Song, Junhua, Zhou, Hua, Du, Dan, Beckman, Scott P., Su, Dong, and Lin, Yuehe. Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MNx Active Moieties Enable Enhanced ORR Performance. United States: N. p., 2018. Web. doi:10.1002/aenm.201801956.
Zhu, Chengzhou, Shi, Qiurong, Xu, Bo Z., Fu, Shaofang, Wan, Gang, Yang, Ce, Yao, Siyu, Song, Junhua, Zhou, Hua, Du, Dan, Beckman, Scott P., Su, Dong, & Lin, Yuehe. Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MNx Active Moieties Enable Enhanced ORR Performance. United States. doi:10.1002/aenm.201801956.
Zhu, Chengzhou, Shi, Qiurong, Xu, Bo Z., Fu, Shaofang, Wan, Gang, Yang, Ce, Yao, Siyu, Song, Junhua, Zhou, Hua, Du, Dan, Beckman, Scott P., Su, Dong, and Lin, Yuehe. Tue . "Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MNx Active Moieties Enable Enhanced ORR Performance". United States. doi:10.1002/aenm.201801956. https://www.osti.gov/servlets/purl/1491129.
@article{osti_1491129,
title = {Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MNx Active Moieties Enable Enhanced ORR Performance},
author = {Zhu, Chengzhou and Shi, Qiurong and Xu, Bo Z. and Fu, Shaofang and Wan, Gang and Yang, Ce and Yao, Siyu and Song, Junhua and Zhou, Hua and Du, Dan and Beckman, Scott P. and Su, Dong and Lin, Yuehe},
abstractNote = {The great interest in fuel cells inspires a substantial amount of research on nonprecious metal catalysts as alternatives to Pt-based oxygen reduction reaction (ORR) electrocatalysts. In this work, bimodal template-based synthesis strategies are proposed for the scalable preparation of hierarchically porous M-N-C (M = Fe or Co) single-atom electrocatalysts featured with active and robust MN2 active moieties. Multiscale tuning of M-N-C catalysts regarding increasing the number of active sites and boosting the intrinsic activity of each active site is realized simultaneously at a single-atom scale. In addition to the antipoisoning power and high affinity for O2, the optimized Fe-N-C catalysts with FeN2 active site presents a superior electrocatalytic activity for ORR with a half-wave potential of 0.927 V (vs reversible hydrogen electrode (RHE)) in an alkaline medium, which is 49 and 55 mV higher than those of the Co-N-C counterpart and commercial Pt/C, respectively. Density functional theory calculations reveal that the FeN2 site is more active than the CoN2 site for ORR due to the lower energy barriers of the intermediates and products involved. In conclusion, the present work may help rational design of more robust ORR electrocatalysts at the atomic level, realizing the significant advances in electrochemical conversion and storage devices.},
doi = {10.1002/aenm.201801956},
journal = {Advanced Energy Materials},
issn = {1614-6832},
number = 29,
volume = 8,
place = {United States},
year = {2018},
month = {8}
}

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