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Enhancing oxygen reduction activity of dinuclear copper complexes loaded on an N-doped carbon support a low-temperature pyrolysis strategy

Bioinspired by the active sites of multicopper oxidases (MCOs), bi/multinuclear copper complexes have attracted great attention in promoting catalytic activity for the oxygen reduction reaction (ORR). Herein, we report the preparation of a Cu-N-C electrocatalyst Cu-BPOZ@CNB-400 for efficient ORR, wh...

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Published in:Dalton transactions : an international journal of inorganic chemistry 2024-07, Vol.53 (27), p.11464-11469
Main Authors: Chi, Hua-Min, Yang, Kun-Zu, Guo, Peng-Peng, Xu, Ying, Xu, Chao, Su, Yong-Zhi, Liu, Xin, Liu, Jin-Gang
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Summary:Bioinspired by the active sites of multicopper oxidases (MCOs), bi/multinuclear copper complexes have attracted great attention in promoting catalytic activity for the oxygen reduction reaction (ORR). Herein, we report the preparation of a Cu-N-C electrocatalyst Cu-BPOZ@CNB-400 for efficient ORR, which was obtained by low temperature pyrolysis of a dinuclear 2,5-bis(2-pyridyl)-1,3,4-oxadiazole (BPOZ) copper complex loaded on a N-doped carbon support at 400 °C. Cu-BPOZ@CNB-400 exhibited a half-wave potential ( E 1/2 ) of 0.86 V vs. RHE for the ORR in 0.1 M KOH solution, which was significantly higher than that of the Cu-BPOZ@CNB-800 ( E 1/2 = 0.83 V) catalyst treated under high temperature (at 800 °C) and the control catalyst Cu-Phen@CNB-400 ( E 1/2 = 0.82 V) derived from low-temperature-treatment (at 400 °C) of a mononuclear phenanthroline-coordinated-Cu complex loaded on a N-doped carbon support. When Cu-BPOZ@CNB-400 was applied as the cathode catalyst in zinc-air batteries a maximum power density ( P max ) of 127 mW cm −2 could be achieved, demonstrating comparable catalyst performance to the commercial 20 wt% Pt/C ( P max = 122 mW cm −2 ) and the control Cu-Phen@CNB-400 catalyst ( P max = 105 mW cm −2 ) under similar experimental conditions. Low-temperature pyrolysis of dinuclear copper complexes on a carbon support improved the charge transfer efficiency, inhibited metal aggregation, and could produce highly dispersed Cu-N-C catalysts with dinuclear copper sites for promoting the 4e − -reduction selectivity of the ORR. It thus provides a cost-effective approach for the controllable fabrication of efficient ORR catalysts to be applied for energy conversion devices. Low-temperature pyrolysis of a dinuclear copper complex loaded on a N-doped carbon support produced an atomically dispersed catalyst with dense active sites that exhibited remarkably enhanced performance for oxygen reduction reaction.
ISSN:1477-9226
1477-9234
DOI:10.1039/d4dt01044b