期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 285, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119861
关键词
Plasma; Single-atom catalyst; Coordination; Platinum; Hydrogen evolution
资金
- National Natural Science Foundation of China [21872098]
The study demonstrates the tunability of Pt single atoms coordination through a cold-plasma technique and predicts a strong correlation between Pt-N coordination concentration and adsorption free energy of H* atoms for the hydrogen evolution reaction (HER). The sample with N, O co-dopant introduced by air plasma shows significantly enhanced performance, with a high turnover frequency and outstanding mass activity, suggesting that the optimized electronic structure of active carbon site plays a key role in improving the catalyst's efficiency.
Coordination tunability of the single-atom catalysts (SACs) is an essential but challenging issue for the catalyst sifting and structure-activity relationship analysis. Herein, Pt single atoms with tunable coordination are readily achieved via a facile cold-plasma technique by changing the gas type (N-2, Ar, or Air) and treatment duration. Combining with density functional theory calculation, the Pt-N coordination concentration is predicted to be highly correlated with adsorption free energy of H* atoms (Delta G(H*)) for the hydrogen evolution reaction (HER), which is further validated experimentally. Remarkably, the sample with N, O co-dopant introduced by air plasma exhibits a high TOF of similar to 13 H-2 s(-1) at 40 mV, and outstanding mass activity of 7.41 A mg(Pt)(-1) for HER, which is 26.5 times of commercial Pt/C catalyst. The enhanced performance might originate from the optimized electronic structure of active carbon site with moderate electron transfer and p-band center, which enables a suitable binding strength with H* and thus a near-zero Delta G(H*).
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