The suppression of the recombination of electrons and holes(e–h) and the enhancement of the light absorption of semiconductors are two key points toward efficient photocatalytic degradation.Here,we report a few-layer...The suppression of the recombination of electrons and holes(e–h) and the enhancement of the light absorption of semiconductors are two key points toward efficient photocatalytic degradation.Here,we report a few-layer g-C_3N_4/α-MoO_3 nanoneedles(flg-C_3N_4/α-MoO_3 NNs) all-solid-state Z-scheme mechanism photocatalyst synthesized via a typical hydrothermal method in a controlled manner.The recombination of the photo-induced e–h pairs could be effectively restrained by the Z-scheme passageway between the flg-C_3N_4 and α-MoO_3 NNs in the composite,which could also promise a high redox ability to degrade pollutants.And it became possible for the prepared photocatalyst to absorb light in a wide range of wavelengths.The detailed mechanism was studied by electron spin-resonance spectroscopy(ESR).The low-dimensional nanostructure of the two constituents(α-MoO_3 NNs with one-dimensional structure and flg-C_3N_4 with two-dimensional structure) endowed the composite with varieties of excellent physicochemical properties,which facilitated the transfer and diffusion of the photoelectrons and increased the specific surface area and the active sites.The 10 wt% flg-C_3N_4/α-MoO_3 NNs showed the best photocatalytic performance toward RhB degradation,the rate of which was 71.86%,~2.6 times higher than that ofα-MoO_3 NNs.展开更多
Crystalline α-MoO3 belts consisting of nanosheets stacked along their [010] axes were synthesized via thermal vapor transport of MoO3 powders at elevated temperatures. The MoO3 belts were millimeters in length along ...Crystalline α-MoO3 belts consisting of nanosheets stacked along their [010] axes were synthesized via thermal vapor transport of MoO3 powders at elevated temperatures. The MoO3 belts were millimeters in length along their [001] axes and tens to hundreds of micrometers in width along their [100] axes. Mechanical and aqueous exfoliations of the belts to form two-dimensional (2D) nanosheets were processed via the scotch-tape and bovine serum albumin (BSA) assisted methods, respectively. Upon scotch-tape exfoliation, the Raman features of MoO3 exhibited monotonic decreases in intensity as the thickness was gradually fell to approach that of a 2D nanosheet. Most Raman features eventually disappeared when a monolayer nanosheet was produced, except for the Mo-O-Mo stretching mode (Ag) at - 818 cm^-1, which was accompanied by mode-softening of up to 5 cm^-1 This mode softening, hitherto not reported for 2D α-MoO3 nanosheets, can be attributed to lattice relaxations that are validated here via theoretical density functional perturbation theory calculations. The BSA-assisted exfoliation products exhibited a blueshift in the α-MoO3 nanosheet absorption edge; they also revealed an absorption peak at 3.98 eV that can be attributed to their intrinsic exciton absorptions. These observations, together with the facile synthesis of high-purity α-MoO3 crystals, illuminate the possibility of further 2D α-MoO3 nanosheet production and lattice dynamic studies.展开更多
基金supported by National Natural Science Foundation of China (21476097,21776118,21507046)Six Talent Peaks Project in Jiangsu Province (2014-JNHB-014)the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘The suppression of the recombination of electrons and holes(e–h) and the enhancement of the light absorption of semiconductors are two key points toward efficient photocatalytic degradation.Here,we report a few-layer g-C_3N_4/α-MoO_3 nanoneedles(flg-C_3N_4/α-MoO_3 NNs) all-solid-state Z-scheme mechanism photocatalyst synthesized via a typical hydrothermal method in a controlled manner.The recombination of the photo-induced e–h pairs could be effectively restrained by the Z-scheme passageway between the flg-C_3N_4 and α-MoO_3 NNs in the composite,which could also promise a high redox ability to degrade pollutants.And it became possible for the prepared photocatalyst to absorb light in a wide range of wavelengths.The detailed mechanism was studied by electron spin-resonance spectroscopy(ESR).The low-dimensional nanostructure of the two constituents(α-MoO_3 NNs with one-dimensional structure and flg-C_3N_4 with two-dimensional structure) endowed the composite with varieties of excellent physicochemical properties,which facilitated the transfer and diffusion of the photoelectrons and increased the specific surface area and the active sites.The 10 wt% flg-C_3N_4/α-MoO_3 NNs showed the best photocatalytic performance toward RhB degradation,the rate of which was 71.86%,~2.6 times higher than that ofα-MoO_3 NNs.
文摘Crystalline α-MoO3 belts consisting of nanosheets stacked along their [010] axes were synthesized via thermal vapor transport of MoO3 powders at elevated temperatures. The MoO3 belts were millimeters in length along their [001] axes and tens to hundreds of micrometers in width along their [100] axes. Mechanical and aqueous exfoliations of the belts to form two-dimensional (2D) nanosheets were processed via the scotch-tape and bovine serum albumin (BSA) assisted methods, respectively. Upon scotch-tape exfoliation, the Raman features of MoO3 exhibited monotonic decreases in intensity as the thickness was gradually fell to approach that of a 2D nanosheet. Most Raman features eventually disappeared when a monolayer nanosheet was produced, except for the Mo-O-Mo stretching mode (Ag) at - 818 cm^-1, which was accompanied by mode-softening of up to 5 cm^-1 This mode softening, hitherto not reported for 2D α-MoO3 nanosheets, can be attributed to lattice relaxations that are validated here via theoretical density functional perturbation theory calculations. The BSA-assisted exfoliation products exhibited a blueshift in the α-MoO3 nanosheet absorption edge; they also revealed an absorption peak at 3.98 eV that can be attributed to their intrinsic exciton absorptions. These observations, together with the facile synthesis of high-purity α-MoO3 crystals, illuminate the possibility of further 2D α-MoO3 nanosheet production and lattice dynamic studies.