Defect-stabilized platinum single atoms and clusters in bilayer nitrogen-doped porous carbon nanocages for synergistic catalysis of basic hydrogen evolution. (5th January 2023)

• Record Type: Journal Article
• Authors: Wang, Chao; Chen, Feiran; Wang, Qinru; Yang, Xiaofeng; Zang, Hu; Yu, Nan; Geng, Baoyou
• Is Part Of: Carbon. Volume 201(2023)
• Page Start: 278
• Page End: 284
• Publication Date: 2023-01-05
• Subjects: Nitrogen-doped porous carbon -- Single atoms -- Synergistic catalysis -- Hygrogen evolution reaction; Carbon -- Periodicals; Carbone -- Périodiques; Koolstof; Toepassingen; Electronic journals; 546.681
• DOI: 10.1016/j.carbon.2022.09.018
• Languages: English
• ISSNs: 0008-6223

Abstract

Abstract: 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. Graphical abstract: Double-layer N-doped carbon nanocages were obtained by ZIF-8, and Pt single atoms and clusters were simultaneously loaded for alkaline HER catalysis. The synergistic catalysis of single atoms and clusters enables its TOF and mass activity to be 5 times and 7.2 times higher than that of commercial Pt/C, respectively. Image 1 Highlights: MOFs-derived bilayer N-doped porous carbon nanocages for co-loading of Pt single atoms and clusters. The turnover frequency (TOF) and mass activity of NPCN–Pt are 5 and 7.2 times higher than those of Pt/C, respectively. Pt single atoms and clusters have a synergistic effect on catalyzing alkaline HER.