Identifying the Key Role of Pyridinic‐N–Co Bonding in Synergistic Electrocatalysis for Reversible ORR/OER
For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g., nitrogen‐doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose e...
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| Published in | Advanced materials (Weinheim) Vol. 30; no. 23; pp. e1800005 - n/a |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Germany
Wiley Subscription Services, Inc
01.06.2018
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0935-9648 1521-4095 1521-4095 |
| DOI | 10.1002/adma.201800005 |
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| Abstract | For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g., nitrogen‐doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM–N–C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo2O4 NPs/N‐doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic‐NCo bonding, instead of pyrrolic‐N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG‐270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn–air battery, NiCo/NLG‐270 exhibits superior charge/discharge performance and long‐term durability compared to the noble metal electrocatalysts.
An innovative strategy based on laser irradiation is developed to selectively regulate relative contents of pyridinic and pyrrolic nitrogen in NiCo2O4/N‐graphene hybrids. Strong chemical bonding forms between nitrogen and cobalt, and pyridinic‐NCo bonds, instead of pyrrolic‐NCo bonds, are identified to predominantly contribute to synergistic catalysis, leading to substantially enhanced oxygen electrocatalytic activities, outperforming a combination of benchmark noble metal catalysts. |
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| AbstractList | For many regenerative electrochemical energy-conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom-doped (e.g., nitrogen-doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM-N-C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo
O
NPs/N-doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic-NCo bonding, instead of pyrrolic-N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG-270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn-air battery, NiCo/NLG-270 exhibits superior charge/discharge performance and long-term durability compared to the noble metal electrocatalysts. For many regenerative electrochemical energy-conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom-doped (e.g., nitrogen-doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM-N-C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo2 O4 NPs/N-doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic-NCo bonding, instead of pyrrolic-N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG-270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn-air battery, NiCo/NLG-270 exhibits superior charge/discharge performance and long-term durability compared to the noble metal electrocatalysts.For many regenerative electrochemical energy-conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom-doped (e.g., nitrogen-doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM-N-C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo2 O4 NPs/N-doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic-NCo bonding, instead of pyrrolic-N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG-270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn-air battery, NiCo/NLG-270 exhibits superior charge/discharge performance and long-term durability compared to the noble metal electrocatalysts. For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g., nitrogen‐doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM–N–C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo2O4 NPs/N‐doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic‐NCo bonding, instead of pyrrolic‐N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG‐270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn–air battery, NiCo/NLG‐270 exhibits superior charge/discharge performance and long‐term durability compared to the noble metal electrocatalysts. An innovative strategy based on laser irradiation is developed to selectively regulate relative contents of pyridinic and pyrrolic nitrogen in NiCo2O4/N‐graphene hybrids. Strong chemical bonding forms between nitrogen and cobalt, and pyridinic‐NCo bonds, instead of pyrrolic‐NCo bonds, are identified to predominantly contribute to synergistic catalysis, leading to substantially enhanced oxygen electrocatalytic activities, outperforming a combination of benchmark noble metal catalysts. For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g., nitrogen‐doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM–N–C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo2O4 NPs/N‐doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic‐NCo bonding, instead of pyrrolic‐N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG‐270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different ΔE among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn–air battery, NiCo/NLG‐270 exhibits superior charge/discharge performance and long‐term durability compared to the noble metal electrocatalysts. For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g., nitrogen‐doped) carbonaceous materials are promising bifunctional oxygen reduction reaction/oxygen evolution reaction electrocatalysts, whose enhanced electrocatalytic activities are attributed to the synergistic effect originated from the TM–N–C active sites. However, it is still ambiguous which configuration of nitrogen dopants, either pyridinic or pyrrolic N, when bonded to the TM in oxides, predominately contributes to the synergistic effect. Herein, an innovative strategy based on laser irradiation is described to controllably tune the relative concentrations of pyridinic and pyrrolic nitrogen dopants in the hybrid catalyst, i.e., NiCo 2 O 4 NPs/N‐doped mesoporous graphene. Comparative studies reveal the dominant role of pyridinic‐NCo bonding, instead of pyrrolic‐N bonding, in synergistically promoting reversible oxygen electrocatalysis. Moreover, density functional theory calculations provide deep insights into the corresponding synergistic mechanism. The optimized hybrid, NiCo/NLG‐270, manifests outstanding reversible oxygen electrocatalytic activities, leading to an overpotential different Δ E among the lowest value for highly efficient bifunctional catalysts. In a practical reversible Zn–air battery, NiCo/NLG‐270 exhibits superior charge/discharge performance and long‐term durability compared to the noble metal electrocatalysts. |
| Author | Liu, Zi‐Wei Luo, Jun Han, Xiao‐Peng Wang, Xue‐Rui Liu, Jie‐Yu Yang, Jing Wang, Wei‐Chao Qiao, Shi‐Zhang Du, Xi‐Wen |
| Author_xml | – sequence: 1 givenname: Xue‐Rui surname: Wang fullname: Wang, Xue‐Rui organization: Tianjin University – sequence: 2 givenname: Jie‐Yu surname: Liu fullname: Liu, Jie‐Yu organization: Nankai University – sequence: 3 givenname: Zi‐Wei surname: Liu fullname: Liu, Zi‐Wei organization: Tianjin University – sequence: 4 givenname: Wei‐Chao surname: Wang fullname: Wang, Wei‐Chao email: weichaowang@nankai.edu.cn organization: Nankai University – sequence: 5 givenname: Jun surname: Luo fullname: Luo, Jun organization: Tianjin University of Technology – sequence: 6 givenname: Xiao‐Peng surname: Han fullname: Han, Xiao‐Peng organization: School of Materials Science and Engineering Tianjin University – sequence: 7 givenname: Xi‐Wen surname: Du fullname: Du, Xi‐Wen organization: Tianjin University – sequence: 8 givenname: Shi‐Zhang surname: Qiao fullname: Qiao, Shi‐Zhang organization: The University of Adelaide – sequence: 9 givenname: Jing orcidid: 0000-0002-3731-368X surname: Yang fullname: Yang, Jing email: yang_jing@tju.edu.cn organization: Tianjin University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/29675934$$D View this record in MEDLINE/PubMed |
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| Snippet | For many regenerative electrochemical energy‐conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom‐doped (e.g.,... For many regenerative electrochemical energy-conversion systems, hybrid electrocatalysts comprising transition metal (TM) oxides and heteroatom-doped (e.g.,... |
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| SubjectTerms | Batteries Bonding Carbonaceous materials Catalysis Catalysts Density functional theory Dopants Electrocatalysis Electrocatalysts graphenes hybrid electrocatalysts Hybrid systems Materials science Metal air batteries Nitrogen Noble metals Oxygen evolution reactions Oxygen reduction reactions pyridinic nitrogen pyrrolic nitrogen spinels Synergistic effect Zinc-oxygen batteries |
| Title | Identifying the Key Role of Pyridinic‐N–Co Bonding in Synergistic Electrocatalysis for Reversible ORR/OER |
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