Main Group SnN 4 O Single Sites with Optimized Charge Distribution for Boosting the Oxygen Reduction Reaction.

Autor: Shao X; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea., Gan R; Tianjin Municipal Key Lab of Advanced Fiber and Energy Storage Technology, Tiangong University, Tianjin 300387, China., Rao Y; College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, China., Nga TTT; Department of Physics, Tamkang University, Taipei, New Taipei City 25137, Taiwan., Liang M; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea., Dong CL; Department of Physics, Tamkang University, Taipei, New Taipei City 25137, Taiwan., Ma C; Tianjin Municipal Key Lab of Advanced Fiber and Energy Storage Technology, Tiangong University, Tianjin 300387, China., Lee JY; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea., Li H; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea., Lee H; Department of Chemistry, Sungkyunkwan University, Suwon 16419, Republic of Korea.; Creative Research Institute, Sungkyunkwan University, Suwon 16419, Republic of Korea.; Institute of Quantum Biophysics, Sungkyunkwan University, Suwon 16419, Republic of Korea.
Jazyk: angličtina
Zdroj: ACS nano [ACS Nano] 2024 Jun 04; Vol. 18 (22), pp. 14742-14753. Date of Electronic Publication: 2024 May 21.
DOI: 10.1021/acsnano.4c04112
Abstrakt: Transition metal single-atom catalysts (SACs) have been regarded as possible alternatives to platinum-based materials due to their satisfactory performance of the oxygen reduction reaction (ORR). By contrast, main-group metal elements are rarely studied due to their unfavorable surface and electronic states. Herein, a main-group Sn-based SAC with penta-coordinated and asymmetric first-shell ligands is reported as an efficient and robust ORR catalyst. The introduction of the vertical oxygen atom breaks the symmetric charge balance, modulating the binding strength to oxygen intermediates and decreasing the energy barrier for the ORR process. As expected, the prepared Sn SAC exhibits outstanding ORR activity with a high half-wave potential of 0.912 V (vs RHE) and an excellent mass activity of 13.1 A mg Sn -1 at 0.850 V (vs RHE), which surpasses that of commercial Pt/C and most reported transition-metal-based SACs. Additionally, the reported Sn SAC shows excellent ORR stability due to the strong interaction between Sn sites and the carbon support with oxygen atom as the bridge. The excellent ORR performance of Sn SAC was also proven by both liquid- and solid-state zinc-air battery (ZAB) measurements, indicating its great potential in practical applications.
Databáze: MEDLINE