Regulating the Coordination Geometry and Oxidation State of Single‐Atom Fe Sites for Enhanced Oxygen Reduction Electrocatalysis

FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts contain...

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Published inSmall (Weinheim an der Bergstrasse, Germany) Vol. 19; no. 24; pp. e2300373 - n/a
Main Authors Wang, Minjie, Wang, Li, Li, Qingbin, Wang, Dan, Yang, Liu, Han, Yongjun, Ren, Yuan, Tian, Gang, Zheng, Xiaoyang, Ji, Muwei, Zhu, Caizhen, Peng, Lishan, Waterhouse, Geoffrey I. N.
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 01.06.2023
Subjects
Catalysts
Chemical reduction
Coordination
Density functional theory
Desorption
Electrolytic cells
Fe coordination geometry
Fe single atoms
FeN x sites
Metal air batteries
Nanotechnology
Open circuit voltage
Oxidation
oxygen reduction reaction
Oxygen reduction reactions
Polypyrroles
Proton exchange membrane fuel cells
Valence
Zinc-oxygen batteries
zinc–air batteries
oxygen reduction reaction
Fe single atoms
FeN x sites
zinc-air batteries
Fe coordination geometry
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Abstract FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3, FeN4, and FeN5 coordinations are synthesized by carbonization of Fe‐rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH− desorption in the rate‐limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state‐of‐the‐art performance (an open circuit potential of 1.629 V, power density of 159 mW cm−2). Results confirm an intimate structure‐activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts. FeNC catalysts with different Fe single‐atom coordination geometries (FeN3, FeN4, or FeN5) are synthesized by pyrolysis of Fe‐polypyrrole precursors. FeN5 sites offer the highest Fe oxidation state (+2.62), strongest Fe–N interaction, lowest energy barrier for OH− desorption, and highest intrinsic activity for oxygen reduction reaction in alkaline media.
AbstractList FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3, FeN4, and FeN5 coordinations are synthesized by carbonization of Fe‐rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH− desorption in the rate‐limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state‐of‐the‐art performance (an open circuit potential of 1.629 V, power density of 159 mW cm−2). Results confirm an intimate structure‐activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.
FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn-air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3 , FeN4 , and FeN5 coordinations are synthesized by carbonization of Fe-rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH- desorption in the rate-limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state-of-the-art performance (an open circuit potential of 1.629 V, power density of 159 mW cm-2 ). Results confirm an intimate structure-activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn-air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3 , FeN4 , and FeN5 coordinations are synthesized by carbonization of Fe-rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH- desorption in the rate-limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state-of-the-art performance (an open circuit potential of 1.629 V, power density of 159 mW cm-2 ). Results confirm an intimate structure-activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.
FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn-air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN , FeN , and FeN coordinations are synthesized by carbonization of Fe-rich polypyrrole precursors. The FeN sites possess a higher Fe oxidation state (+2.62) than the FeN (+2.23) and FeN (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH desorption in the rate-limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN sites demonstrates state-of-the-art performance (an open circuit potential of 1.629 V, power density of 159 mW cm ). Results confirm an intimate structure-activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.
FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN 3 , FeN 4 , and FeN 5 coordinations are synthesized by carbonization of Fe‐rich polypyrrole precursors. The FeN 5 sites possess a higher Fe oxidation state (+2.62) than the FeN 3 (+2.23) and FeN 4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN 5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH − desorption in the rate‐limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN 5 sites demonstrates state‐of‐the‐art performance (an open circuit potential of 1.629 V, power density of 159 mW cm −2 ). Results confirm an intimate structure‐activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.
FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3, FeN4, and FeN5 coordinations are synthesized by carbonization of Fe‐rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH− desorption in the rate‐limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state‐of‐the‐art performance (an open circuit potential of 1.629 V, power density of 159 mW cm−2). Results confirm an intimate structure‐activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts. FeNC catalysts with different Fe single‐atom coordination geometries (FeN3, FeN4, or FeN5) are synthesized by pyrolysis of Fe‐polypyrrole precursors. FeN5 sites offer the highest Fe oxidation state (+2.62), strongest Fe–N interaction, lowest energy barrier for OH− desorption, and highest intrinsic activity for oxygen reduction reaction in alkaline media.
Author Zheng, Xiaoyang
Wang, Li
Han, Yongjun
Ji, Muwei
Wang, Dan
Waterhouse, Geoffrey I. N.
Ren, Yuan
Yang, Liu
Tian, Gang
Wang, Minjie
Li, Qingbin
Zhu, Caizhen
Peng, Lishan
Author_xml – sequence: 1
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  surname: Wang
  fullname: Wang, Minjie
  organization: Pingdingshan University
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  fullname: Wang, Li
  organization: Pingdingshan University
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  givenname: Qingbin
  surname: Li
  fullname: Li, Qingbin
  email: 3204@pdsu.edu.cn
  organization: Pingdingshan University
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  givenname: Dan
  surname: Wang
  fullname: Wang, Dan
  organization: Pingdingshan University
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  givenname: Liu
  surname: Yang
  fullname: Yang, Liu
  organization: Pingdingshan University
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  givenname: Yongjun
  surname: Han
  fullname: Han, Yongjun
  organization: Pingdingshan University
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  fullname: Ren, Yuan
  organization: Fudan University
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  surname: Tian
  fullname: Tian, Gang
  organization: Pingdingshan University
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  givenname: Xiaoyang
  surname: Zheng
  fullname: Zheng, Xiaoyang
  organization: University of Tsukuba
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  givenname: Muwei
  surname: Ji
  fullname: Ji, Muwei
  organization: Shantou University
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  givenname: Caizhen
  surname: Zhu
  fullname: Zhu, Caizhen
  email: czzhu@szu.edu.cn
  organization: Shenzhen University
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  givenname: Lishan
  surname: Peng
  fullname: Peng, Lishan
  email: lspeng@gia.cas.cn
  organization: The University of Auckland
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  givenname: Geoffrey I. N.
  orcidid: 0000-0002-3296-3093
  surname: Waterhouse
  fullname: Waterhouse, Geoffrey I. N.
  email: g.waterhouse@auckland.ac.nz
  organization: The University of Auckland
BackLink https://www.ncbi.nlm.nih.gov/pubmed/36919312$$D View this record in MEDLINE/PubMed
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Issue 24
Keywords oxygen reduction reaction
Fe single atoms
FeN x sites
zinc-air batteries
Fe coordination geometry
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2023 The Authors. Small published by Wiley-VCH GmbH.
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Snippet FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn–air...
FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn-air...
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StartPage e2300373
SubjectTerms Catalysts
Chemical reduction
Coordination
Density functional theory
Desorption
Electrolytic cells
Fe coordination geometry
Fe single atoms
FeN x sites
Metal air batteries
Nanotechnology
Open circuit voltage
Oxidation
oxygen reduction reaction
Oxygen reduction reactions
Polypyrroles
Proton exchange membrane fuel cells
Valence
Zinc-oxygen batteries
zinc–air batteries
Title Regulating the Coordination Geometry and Oxidation State of Single‐Atom Fe Sites for Enhanced Oxygen Reduction Electrocatalysis
URI https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fsmll.202300373
https://www.ncbi.nlm.nih.gov/pubmed/36919312
https://www.proquest.com/docview/2825384935
https://www.proquest.com/docview/2787212078
Volume 19
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