Identifying the Key Role of Pyridinic-N-Co Bonding in Synergistic Electrocatalysis for Reversible ORR/OER

© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 30(2018), 23 vom: 19. Juni, Seite e1800005
1. Verfasser: Wang, Xue-Rui (VerfasserIn)
Weitere Verfasser: Liu, Jie-Yu, Liu, Zi-Wei, Wang, Wei-Chao, Luo, Jun, Han, Xiao-Peng, Du, Xi-Wen, Qiao, Shi-Zhang, Yang, Jing
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2018
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article graphenes hybrid electrocatalysts pyridinic nitrogen pyrrolic nitrogen spinels
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520 |a © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. 
520 |a 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-NCo 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 
650 4 |a Journal Article 
650 4 |a graphenes 
650 4 |a hybrid electrocatalysts 
650 4 |a pyridinic nitrogen 
650 4 |a pyrrolic nitrogen 
650 4 |a spinels 
700 1 |a Liu, Jie-Yu  |e verfasserin  |4 aut 
700 1 |a Liu, Zi-Wei  |e verfasserin  |4 aut 
700 1 |a Wang, Wei-Chao  |e verfasserin  |4 aut 
700 1 |a Luo, Jun  |e verfasserin  |4 aut 
700 1 |a Han, Xiao-Peng  |e verfasserin  |4 aut 
700 1 |a Du, Xi-Wen  |e verfasserin  |4 aut 
700 1 |a Qiao, Shi-Zhang  |e verfasserin  |4 aut 
700 1 |a Yang, Jing  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Advanced materials (Deerfield Beach, Fla.)  |d 1998  |g 30(2018), 23 vom: 19. Juni, Seite e1800005  |w (DE-627)NLM098206397  |x 1521-4095  |7 nnns 
773 1 8 |g volume:30  |g year:2018  |g number:23  |g day:19  |g month:06  |g pages:e1800005 
856 4 0 |u http://dx.doi.org/10.1002/adma.201800005  |3 Volltext 
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