Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 39, Pages 21237-21241Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202108599
Keywords
main-group metals; oxygen reduction reaction; p-block antimony; single-atom catalyst; Zn-air battery
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Funding
- National Natural Science Foundation of China [52025013, 51922031]
- 111 Project [B12015]
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In this study, a p-block antimony single-atom catalyst with Sb-N-4 configuration was successfully synthesized for efficient catalysis of the oxygen reduction reaction (ORR). The Sb SAC exhibited superior ORR activity and stability compared to most transition-metal based SACs and commercial Pt/C. Experimental and theoretical calculations revealed that the active catalytic sites were positively charged Sb-N-4 single-metal sites, indicating promising potential for the design of highly active main-group-metal SACs.
Main-group (s- and p-block) metals are generally regarded as catalytically inactive due to the delocalized s/p-band. Herein, we successfully synthesized a p-block antimony single-atom catalyst (Sb SAC) with the Sb-N-4 configuration for efficient catalysis of the oxygen reduction reaction (ORR). The obtained Sb SAC exhibits superior ORR activity with a half-wave potential of 0.86 V and excellent stability, which outperforms most transition-metal (TM, d-block) based SACs and commercial Pt/C. In addition, it presents an excellent power density of 184.6 mW cm(-2) and a high specific capacity (803.5 mAh g(-1)) in Zn-air battery. Both experiment and theoretical calculation manifest that the active catalytic sites are positively charged Sb-N-4 single-metal sites, which have closed d shells. Density of states (DOS) results unveil the p orbital of the atomically dispersed Sb cation in Sb SAC can easily interact with O-2-p orbital to form hybrid states, facilitating the charge transfer and generating appropriate adsorption strength for oxygen intermediates, lowering the energy barrier and modulating the rate-determining step. This work sheds light on the atomic-level preparing p-block Sb metal catalyst for highly active ORR, and further provides valuable guidelines for the rational design of other main-group-metal SACs.
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