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

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

doi:10.1002/aenm.201801956

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

Journal Article · Tue Aug 28 00:00:00 EDT 2018 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201801956· OSTI ID:1491129

Zhu, Chengzhou ^[1]; Shi, Qiurong ^[2]; Xu, Bo Z. ^[3]; Fu, Shaofang ^[2]; Wan, Gang ^[4]; Yang, Ce ^[4]; Yao, Siyu ^[5]; Song, Junhua ^[2]; Zhou, Hua ^[4]; Du, Dan ^[1]; Beckman, Scott P. ^[2]; Su, Dong ^[5];

^[2]

Washington State Univ., Pullman, WA (United States); Central China Normal Univ., Wuhan (People's Republic of China)
Washington State Univ., Pullman, WA (United States)
Univ. of California, Berkeley, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 1491129

Alternate ID(s):: OSTI ID: 1467735; OSTI ID: 1484234

Report Number(s):: BNL-210876-2019-JAAM

Journal Information:: Advanced Energy Materials, Vol. 8, Issue 29; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 464 works

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Self-templated nitrogen-doped mesoporous carbon decorated with double transition-metal active sites for enhanced oxygen electrode catalysis Qiao, Meng-Fei; Wang, Ying; Li, Lei Rare Metals, Vol. 39, Issue 7 https://doi.org/10.1007/s12598-019-01345-9	journal	December 2019
Transition Metal‐Nitrogen‐Carbon Active Site for Oxygen Reduction Electrocatalysis: Beyond the Fascinations of TM‐N₄ Zhang, Cai; Zhang, Wei; Zheng, Weitao ChemCatChem, Vol. 11, Issue 2 https://doi.org/10.1002/cctc.201801679	journal	November 2018
Tailoring FeN ₄ Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell Fu, Xiaogang; Li, Na; Ren, Bohua Advanced Energy Materials, Vol. 9, Issue 11 https://doi.org/10.1002/aenm.201803737	journal	January 2019
MOF nanoleaves as new sacrificial templates for the fabrication of nanoporous Co–N _x /C electrocatalysts for oxygen reduction Li, Jingjing; Xia, Wei; Tang, Jing Nanoscale Horizons, Vol. 4, Issue 4 https://doi.org/10.1039/c9nh00095j	journal	January 2019
A review of non-precious metal single atom confined nanomaterials in different structural dimensions (1D–3D) as highly active oxygen redox reaction electrocatalysts Liu, Jin; Zhang, Hao; Qiu, Ming Journal of Materials Chemistry A, Vol. 8, Issue 5 https://doi.org/10.1039/c9ta11852g	journal	January 2020
A Single‐Atom Iridium Heterogeneous Catalyst in Oxygen Reduction Reaction Xiao, Meiling; Zhu, Jianbing; Li, Gaoran Angewandte Chemie, Vol. 131, Issue 28 https://doi.org/10.1002/ange.201905241	journal	June 2019
Single-atom catalysts for electrochemical clean energy conversion: recent progress and perspectives Li, Huining; Zhu, Han; Zhuang, Zechao Sustainable Energy & Fuels, Vol. 4, Issue 3 https://doi.org/10.1039/c9se01004a	journal	January 2020
Electrosynthesis of Hydrogen Peroxide Synergistically Catalyzed by Atomic Co–N _x –C Sites and Oxygen Functional Groups in Noble‐Metal‐Free Electrocatalysts Li, Bo‐Quan; Zhao, Chang‐Xin; Liu, Jia‐Ning Advanced Materials, Vol. 31, Issue 35 https://doi.org/10.1002/adma.201808173	journal	April 2019
When Nanozymes Meet Single‐Atom Catalysis Jiao, Lei; Yan, Hongye; Wu, Yu Angewandte Chemie, Vol. 132, Issue 7 https://doi.org/10.1002/ange.201905645	journal	October 2019
Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN ₄ for Ultraefficient Oxygen Reduction Reaction in Proton‐Exchange Membrane Fuel Cells Qiao, Mengfei; Wang, Ying; Wang, Quan Angewandte Chemie International Edition, Vol. 59, Issue 7 https://doi.org/10.1002/anie.201914123	journal	February 2020
Electrosynthesis of Hydrogen Peroxide Synergistically Catalyzed by Atomic Co–N _x –C Sites and Oxygen Functional Groups in Noble‐Metal‐Free Electrocatalysts Li, Bo‐Quan; Zhao, Chang‐Xin; Liu, Jia‐Ning Advanced Materials, Vol. 31, Issue 35 https://doi.org/10.1002/adma.201904044	journal	July 2019

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29 ENERGY PLANNING
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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