Defect-stabilized platinum single atoms and clusters in bilayer nitrogen-doped porous carbon nanocages for synergistic catalysis of basic hydrogen evolution
2023
Wang, Chao | Chen, Feiran | Wang, Qinru | Yang, Xiaofeng | Zang, Hu | Yu, Nan | Geng, Baoyou
Alkaline water electrolysis is a safe and efficient method for producing hydrogen that is favored by the industry. At present, single-atom catalysts have attracted extensive attention due to their extremely high atom utilization. However, studies on the single-atom site catalytic mechanism of the Volmer step, the rate-determining step of the cathodic HER reaction, are lacking. Here, we used ZIF-8 to obtain double-layer N-doped porous carbon nanocages, and successfully achieved the co-loading of Pt single atoms and their clusters (NPCN–Pt). The turnover frequency (TOF) and mass activity of NPCN–Pt are 5 and 7.2 times higher than those of commercial Pt/C, respectively, and the former exhibits significantly better stability than Pt/C. Theoretical calculations show that Pt clusters have a lower activation energy barrier for water molecules compared to Pt single atoms, which favors the Volmer step. The ΔGH* of Pt single-atom sites is smaller than that of Pt clusters, which is more conducive to the release of H₂. The study shows that Pt clusters and single atoms can synergistically catalyze the HER reaction, providing new ideas for the development of efficient HER catalysts.
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