摘要
The development of high-performance metal single-atom catalysts(SACs)for HCOOH dehydrogenation offers a viable strategy for H_(2) production in fuel cells.Using density functional theory(DFT)calculations,we systematically investigated the HCOOH dehydrogenation on the single Pt and Pd atom embedded in monovacancy defective graphene(PtG and PdG).We found that both PtG and PdG exhibited good stability and activity.Additionally,the C-H bond activation pathway was more energetically favorable than that of O-H bond activation of the two catalyzed reactions.Further,PtG possessed higher activity for HCOOH dehydrogenation than PdG due to the upshift of the d-orbital center(-3.68 vs-3.88 eV).These findings provide new insights into the rational design of SACs for HCOOH dehydrogenation.
基金
supported by the National Natural Science Foundation of China(grant nos.21963007 and 22473039)
the Natural Science Foundation and the Excellent Youth Foundation of Shandong Province,China(grant nos.ZR2020MB048,ZR2021MB023,and ZR2022YQ16)
the Fundamental Research Fund of Henan Academy of Sciences,China(grant no.240626058).
