Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil i...Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil in glycerol solution containing fluorinion and 20%deionized water. Subsequently, g-C_3N_4 film was hydrothermally grown on TNTAs via the hydrogen-bonded cyanuric acid melamine supramolecular complex. The results showed that g-C_3N_4 was successfully decorated on the TNTAs and the g-C_3N_4/TNTAs served as an efficient and stable photoanode for photoelectrochemical water splitting. The facile deposition method enables the fabrication of efficient and low-cost photoanodes for renewable energy applications.展开更多
The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on th...The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on the surface of regular Bi_4Ti_3O_(12) sheets. Comparing with pure Bi_4Ti_3O_(12) and g-C_3N_4, the Bi_4Ti_3O_(12)/g-C_3N_4 composites showed significant enhancement in photocatalytic efficiency for the degradation of RhB in solution. With the mass ratio of g-C_3N_4 increasing to 10 wt%, the Bi_4Ti_3O_(12)/g-C_3N_4-10% presented the best photocatalytic activity. Its photocatalysis reaction constant was approximately 2 times higher than the single component Bi_4Ti_3O_(12) or g-C_3N_4. Meanwhile, good stability and durability for the Bi_4Ti_3O_(12)/g-C_3N_4-10% were confirmed by the recycling experiment and FT-IR analysis. The possible mechanism for the improvements was the matched band positions and the effective separation of photo-excited electrons(e-) and holes(h+). Furthermore, based on the results of active species trapping, photo-generated holes(h+) and superoxide radical(·O2-) could be the main radicals in reaction.展开更多
MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3...MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3N_4 and MoS_2 nanosheets. The effects of MoS_2 content on the light absorption, charge transfer and photocatalytic activity of the hybrid samples were investigated. Characterization results show that MoS_2 nanosheets are well anchored on the face of C_3N_4 nanosheets and the composites have well dispersed layered morphology. After loading with MoS_2, the light absorption of composites was much improved, especially in visible-light region. The photocatalytic activities of C_3N_4/MoS_2 samples were evaluated based on the H_2 evolution under visible light irradiation(λ > 400 nm). When the loading amount of MoS_2 was increased to 5 wt%, the highest H_2 evolution rate(274 μmol·g^(-1)·h^(-1)) was obtained. Compared with samples obtained from direct impregnation method, sonication pretreatment is favorable for the formation of 2D layered heterojuctions and thus improve the photocatalytic activity. Slightly deactivation of C_3N_4/MoS_2 composites could be observed when recycled due to the mild photocorrosion of MoS_2. Based on the band alignments of C_3N_4 and MoS_2, a possible photocatalytic mechanism was discussed, where MoS_2 could efficiently promote the separation of the photogenerated carriers of C_3N_4.展开更多
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
The polycrystalline phase WO_3/g-C_3N_4 was synthesized under stirring using tungstenic acid(H_2WO_4) and graphitic carbon nitride(g-C_3N_4) as raw materials. The catalyst was characterized by X-ray diffraction(XRD), ...The polycrystalline phase WO_3/g-C_3N_4 was synthesized under stirring using tungstenic acid(H_2WO_4) and graphitic carbon nitride(g-C_3N_4) as raw materials. The catalyst was characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),the Fourier transform infrared spectroscopy(FT-IR),and the Brunauer-Emmett-Teller analysis(BET). The polycrystalline phase WO_3/g-C_3N_4 was determined by XRD technique. The oxidative desulfurization process was investigated using WO_3/g-C_3N_4 as the catalyst, 30% hydrogen peroxide(H202) as the oxidant, and 1-butyl-3-methylimidazolium tetrafluoroborate([bmim]BF4) ionic liquids(ILs) as the extractant. The operating conditions, including H_2WO_4 amount, IL dose, H_2 O_2 volume, temperature, catalyst dosage, and types of sulfur compounds,were systematically researched. The desulfurization rate could reach 98.46% for removing dibenzothiophene(DBT) from the model oil under optimal reaction conditions. In addition, the catalytic activity was slightly decreased after five recycles of catalysts. The reaction kinetics analysis shows that the oxidative desulfurization system was in accord with the first-order reaction kinetics equation. The mechanism of oxidative desulfurization was proposed.展开更多
The effect of an external electric field on the bandgap is observed for two proposed heterostructures graphitic carbon nitride-graphene-hexagonal boron nitride(g-C_3N_4/G/h-BN) in hexagonal stack(AAA) and graphene-gra...The effect of an external electric field on the bandgap is observed for two proposed heterostructures graphitic carbon nitride-graphene-hexagonal boron nitride(g-C_3N_4/G/h-BN) in hexagonal stack(AAA) and graphene-graphitic carbon nitridehexagonal boron nitride(G/g-C_3N_4/h-BN) in Bernal stack(ABA). Their inter-layer distance, binding energy and effective mass has also been calculated. The structure optimization has been done by density functional theory(DFT) with van der Waals corrections. The inter-layer distance, bandgap, binding energy and effective mass has been listed for these heterostructures and compared with that of bilayer graphene(BLG), graphene-hexagonal boron nitride(G/h-BN) hetero-bilayer, graphene-graphitic carbon nitride(G/g-C_3N_4) hetero-bilayer and graphitic carbon nitride-graphene-graphitic carbon nitride(g-C_3N_4/G/g-C_3N_4) heterostructure in Bernal and hexagonal stack. g-C_3N_4/G/h-BN is found to offer lower effective mass and larger bandgap opening among the considered heterostructures.展开更多
基金financial support from the National Natural Science Foundation of China (Nos. 51702025, 51574047)Natural Science Foundation of Jiangsu Province (Nos. BK20160277, BK20150259)
文摘Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil in glycerol solution containing fluorinion and 20%deionized water. Subsequently, g-C_3N_4 film was hydrothermally grown on TNTAs via the hydrogen-bonded cyanuric acid melamine supramolecular complex. The results showed that g-C_3N_4 was successfully decorated on the TNTAs and the g-C_3N_4/TNTAs served as an efficient and stable photoanode for photoelectrochemical water splitting. The facile deposition method enables the fabrication of efficient and low-cost photoanodes for renewable energy applications.
基金Supported by the National Natural Science Foundation of China(51509220)the Natural Science Foundation of Zhejiang Province(LQ14E090003)+1 种基金Ningbo Science and Technology Plan Projects(2014C50007,2014C51003)Ningbo major social development projects(2017C510006)
文摘The Bi_4Ti_3O_(12)/g-C_3N_4 composites with microsheet and nanosheet structure were prepared through facile ultrasonic-assisted method. The SEM and TEM results suggested that the nanosheets g-C_3N_4 were stacked on the surface of regular Bi_4Ti_3O_(12) sheets. Comparing with pure Bi_4Ti_3O_(12) and g-C_3N_4, the Bi_4Ti_3O_(12)/g-C_3N_4 composites showed significant enhancement in photocatalytic efficiency for the degradation of RhB in solution. With the mass ratio of g-C_3N_4 increasing to 10 wt%, the Bi_4Ti_3O_(12)/g-C_3N_4-10% presented the best photocatalytic activity. Its photocatalysis reaction constant was approximately 2 times higher than the single component Bi_4Ti_3O_(12) or g-C_3N_4. Meanwhile, good stability and durability for the Bi_4Ti_3O_(12)/g-C_3N_4-10% were confirmed by the recycling experiment and FT-IR analysis. The possible mechanism for the improvements was the matched band positions and the effective separation of photo-excited electrons(e-) and holes(h+). Furthermore, based on the results of active species trapping, photo-generated holes(h+) and superoxide radical(·O2-) could be the main radicals in reaction.
基金Funded by the National Natural Science Foundation of China(No.21503096)
文摘MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3N_4 and MoS_2 nanosheets. The effects of MoS_2 content on the light absorption, charge transfer and photocatalytic activity of the hybrid samples were investigated. Characterization results show that MoS_2 nanosheets are well anchored on the face of C_3N_4 nanosheets and the composites have well dispersed layered morphology. After loading with MoS_2, the light absorption of composites was much improved, especially in visible-light region. The photocatalytic activities of C_3N_4/MoS_2 samples were evaluated based on the H_2 evolution under visible light irradiation(λ > 400 nm). When the loading amount of MoS_2 was increased to 5 wt%, the highest H_2 evolution rate(274 μmol·g^(-1)·h^(-1)) was obtained. Compared with samples obtained from direct impregnation method, sonication pretreatment is favorable for the formation of 2D layered heterojuctions and thus improve the photocatalytic activity. Slightly deactivation of C_3N_4/MoS_2 composites could be observed when recycled due to the mild photocorrosion of MoS_2. Based on the band alignments of C_3N_4 and MoS_2, a possible photocatalytic mechanism was discussed, where MoS_2 could efficiently promote the separation of the photogenerated carriers of C_3N_4.
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.
基金the financial support of the Doctoral Fund of Liaoning Province (201501105)
文摘The polycrystalline phase WO_3/g-C_3N_4 was synthesized under stirring using tungstenic acid(H_2WO_4) and graphitic carbon nitride(g-C_3N_4) as raw materials. The catalyst was characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),the Fourier transform infrared spectroscopy(FT-IR),and the Brunauer-Emmett-Teller analysis(BET). The polycrystalline phase WO_3/g-C_3N_4 was determined by XRD technique. The oxidative desulfurization process was investigated using WO_3/g-C_3N_4 as the catalyst, 30% hydrogen peroxide(H202) as the oxidant, and 1-butyl-3-methylimidazolium tetrafluoroborate([bmim]BF4) ionic liquids(ILs) as the extractant. The operating conditions, including H_2WO_4 amount, IL dose, H_2 O_2 volume, temperature, catalyst dosage, and types of sulfur compounds,were systematically researched. The desulfurization rate could reach 98.46% for removing dibenzothiophene(DBT) from the model oil under optimal reaction conditions. In addition, the catalytic activity was slightly decreased after five recycles of catalysts. The reaction kinetics analysis shows that the oxidative desulfurization system was in accord with the first-order reaction kinetics equation. The mechanism of oxidative desulfurization was proposed.
文摘The effect of an external electric field on the bandgap is observed for two proposed heterostructures graphitic carbon nitride-graphene-hexagonal boron nitride(g-C_3N_4/G/h-BN) in hexagonal stack(AAA) and graphene-graphitic carbon nitridehexagonal boron nitride(G/g-C_3N_4/h-BN) in Bernal stack(ABA). Their inter-layer distance, binding energy and effective mass has also been calculated. The structure optimization has been done by density functional theory(DFT) with van der Waals corrections. The inter-layer distance, bandgap, binding energy and effective mass has been listed for these heterostructures and compared with that of bilayer graphene(BLG), graphene-hexagonal boron nitride(G/h-BN) hetero-bilayer, graphene-graphitic carbon nitride(G/g-C_3N_4) hetero-bilayer and graphitic carbon nitride-graphene-graphitic carbon nitride(g-C_3N_4/G/g-C_3N_4) heterostructure in Bernal and hexagonal stack. g-C_3N_4/G/h-BN is found to offer lower effective mass and larger bandgap opening among the considered heterostructures.
