Cold-plasma technique enabled supported Pt single atoms with tunable coordination for hydrogen evolution reaction

Abstract
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 (N2, 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 (ΔGH*) 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 ∼13 H2 s−1 at 40 mV, and outstanding mass activity of 7.41 A mg−1Pt 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 ΔGH*.

Citation
Li, J., Zhou, Y., Tang, W., Zheng, J., Gao, X., Wang, N., … Chu, W. (2020). Cold-plasma technique enabled supported Pt single atoms with tunable coordination for hydrogen evolution reaction. Applied Catalysis B: Environmental, 119861. doi:10.1016/j.apcatb.2020.119861

Acknowledgements
J. Li, Y. Zhou, and W. Tang contributed equally to this work. We acknowledge the financial support from the National Natural Science Foundation of China (21872098). The State Key Laboratory of Polymer Materials Engineering at Sichuan University is acknowledged for providing Dmol3 modules.

Publisher
Elsevier BV

Journal
Applied Catalysis B: Environmental

DOI
10.1016/j.apcatb.2020.119861

Additional Links
https://linkinghub.elsevier.com/retrieve/pii/S0926337320312789

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