Second-shell modulation on porphyrin-like Pt single atom catalysts for boosting oxygen reduction reaction.

Autor: Najam T; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn.; College of Physics and Optoelectronic Engineering, Shenzhen University Shenzhen 518060 China., Shah SSA; Department of Chemistry, School of Natural Sciences, National University of Sciences and Technology Islamabad 44000 Pakistan., Yin H; QUT Centre for Materials Science, Queensland University of Technology (QUT) 2 George Street Brisbane 4000 Australia., Xiao X; Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM), SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory (SKAEM-JIL), Department of Chemistry and Department of Materials Science and Engineering, Southern University of Science and Technology (SUSTech) Shenzhen 518055 China xuq@sustech.edu.cn., Talib S; Advanced Materials Chemistry Centre (AMCC), SAN Campus, Khalifa University Abu Dhabi P. O. Box 127788 United Arab Emirates., Ji Q; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn., Deng Y; College of Mechatronics and Control Engineering, Shenzhen University Shenzhen 518060 PR China., Javed MS; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn., Hu J; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn., Zhao R; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn., Du A; QUT Centre for Materials Science, Queensland University of Technology (QUT) 2 George Street Brisbane 4000 Australia., Cai X; Institute for Advanced Study, Shenzhen University Shenzhen 518060 China cai.xingke@szu.edu.cn., Xu Q; Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM), SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory (SKAEM-JIL), Department of Chemistry and Department of Materials Science and Engineering, Southern University of Science and Technology (SUSTech) Shenzhen 518055 China xuq@sustech.edu.cn.; Institute for Integrated Cell-Material Sciences (WPI-iCeMS), Kyoto University Yoshida, Sakyo-ku Kyoto 606-8501 Japan.
Jazyk: angličtina
Zdroj: Chemical science [Chem Sci] 2024 Oct 09. Date of Electronic Publication: 2024 Oct 09.
DOI: 10.1039/d4sc03369h
Abstrakt: The first coordination shell is considered crucial in determining the performance of single atom catalysts (SACs), but the significance of the second coordination shell has been overlooked. In this study, we developed a post-doping strategy to realize predictable and controlled modulation on the second coordination shell. By incorporating a P atom into the second coordination shell of a porphyrin-like Pt SAC, the charge density at the Fermi level of Pt single atom increases, enhancing its intrinsic activity. Moreover, the P atom shows stronger adsorption towards large size anions (ClO 4 - ) than Pt atoms, preventing the Pt site poisoning in acid. As a result, the Pt-N 4 P-C catalyst exhibits significantly higher activity than the Pt-N 4 -C catalyst. It even outperforms commercial Pt/C (20 wt% Pt) with a Pt content of only 0.22 wt% in both alkaline and acidic solutions. This work indicates the second coordination shell modulation also greatly impacts the performance of SACs.
Competing Interests: The authors declared no conflict of interest.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE
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