In this paper, N-doped TiO2 mixed crystals are prepared
via direct calcination of TiN for highly selective oxidation of CH4 to HCHO at room temperature. The structures of the prepared
TiO2 samples are characterized to be N-doped TiO2 of anatase and rutile mixed crystals. The crystal structures of
TiO2 samples are determined by XRD spectra and Raman spectra,
while N doping is demonstrated by TEM mapping, ONH inorganic element
analysis, and high-resolution XPS results. Significantly, the production
rate of HCHO is as high as 23.5 mmol·g−1·h−1 with a selectivity over 90%. Mechanism studies reveal
that H2O is the main oxygen source and acts through the
formation of ·OH. DFT calculations indicate that the construction
of a mixed crystal structure and N-doping modification mainly act
by increasing the adsorption capacity of H2O. An efficient
photocatalyst was prepared by us to convert CH4 to HCHO
with high yield and selectivity, greatly promoting the development
of the photocatalytic CH4 conversion study.