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Download fileSingle-Atom Pt–N3 Sites on the Stable Covalent Triazine Framework Nanosheets for Photocatalytic N2 Fixation
journal contribution
posted on 2020-02-03, 12:42 authored by Jian Li, Peng Liu, Yuanzhe Tang, Hongliang Huang, Hongzhi Cui, Donghai Mei, Chongli ZhongThe commercial Haber-Bosch
process for NH3 production
not only requires large amounts of energy and hydrogen supply but
also generates tremendous greenhouse CO2 emission. To mitigate
energy and environmental challenges, renewable ammonia production
technologies based on electrochemical and photochemical methods, in
particular, photocatalytic nitrogen fixation in aqueous phase for
ammonia production is highly desired. In the present work, single-atom
Pt anchored at the −N3 sites of stable and ultrathin
covalent triazine framework (CTF) nanosheets have been successfully
synthesized (Pt-SACs/CTF). The well-defined coordination structure
of Pt–N3 sites in the Pt-SACs/CTF catalyst have
been characterized using HAADF-STEM and EXAFS, as well as ab initio
molecular dynamics simulations. The ammonia production rate over the
as-synthesized Pt-SACs/CTF catalyst is 171.40 μmol g–1 h–1 in the absence of sacrificial agent. On the
basis of density functional theory calculations, it has been found
that the alternating mechanism is energetically more favorable than
the distal mechanism over the well-defined Pt–N3 sites. The significance of the present work is to demonstrate that
the single-atom metal catalysts are anchored at the two-dimensional
stable CTF nanosheets for photocatalytic nitrogen fixation to ammonia.
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Keywords
EXAFSsingle-atom metal catalystsHAADF-STEMNH 3 productionphotocatalytic nitrogen fixationtheory calculationsammonia productiongreenhouse CO 2 emissionStable Covalent Triazine Framework NanosheetsPhotocatalytic N 2 Fixationsingle-atom Ptammonia production technologieshydrogen supplyHaber-Bosch processPt-SACcoordination structuresiteultrathin covalent triazine frameworkmechanismab initiodynamics simulationsCTF nanosheetsammonia production rate