期刊
CARBON
卷 201, 期 -, 页码 278-284出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2022.09.018
关键词
Nitrogen-doped porous carbon; Single atoms; Synergistic catalysis; Hygrogen evolution reaction
This study successfully synthesized NPCN-Pt, which consists of Pt clusters and single atoms loaded on N-doped porous carbon nanocages using ZIF-8 as a catalyst for alkaline water electrolysis. The results showed that NPCN-Pt exhibited significantly higher turnover frequency and mass activity compared to commercial Pt/C, and demonstrated better stability. Theoretical calculations indicated that Pt clusters had a lower activation energy barrier for water molecules compared to Pt single atoms, promoting the Volmer step. Furthermore, Pt single-atom sites had a smaller delta G(H*) than Pt clusters, facilitating the release of H-2. Therefore, the synergistic catalytic effect of Pt clusters and single atoms in the HER reaction provides new insights for the development of efficient HER catalysts.
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 delta G(H*) of Pt single-atom sites is smaller than that of Pt clusters, which is more conducive to the release of H-2. 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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