One-dimensional nickel titanate nanofibers (NiTiO3 NFs) were synthesized and loaded with acetic acid-treated exfoliated and sintered sheets of graphitic carbon nitride (AAs-gC3N4) to fabricate a unique heterogeneous structure. This novel fabrication method for porous AAs-gC3N4 sheets using acetic acid-treated exfoliation followed by sintering provided gC3N4 with a surface area manifold larger than that of bulk gC3N4, with an abundance of catalytically active sites. Hybrid photocatalysts were synthesized through a two-step process. Firstly, NiTiO3 NFs (360 nm in diameter) were made by electrospinning, and these NiTiO3 NFs were sensitized with exfoliated gC3N4 sheets via a sonication process. Varying the weight ratio of NiTiO3 fibers to porous AAs-gC3N4 established that NiTiO3 NFs containing 40 wt% of porous AAs-gC3N4 exhibited optimal activity, i.e., removal of methylene blue and H2 evolution. After 60 min exposure to visible light irradiation, 97% of the methylene blue molecules were removed by the hybrid photocatalyst, compared with 82%, 72%, and 76% by pristine AAs-gC3N4, NiTiO3 NFs, and bulk gC3N4, respectively. The optimal structure also displayed excellent H2 evolution performance. The H2 evolution rate in the optimal sample (152 μmol g−1) was 2.2, 3.2 and 3-fold higher than that in pure AAs-gC3N4 (69 μmol g−1), NiTiO3 NFs (47 μmol g−1) and bulk gC3N4 (50 μmol g−1), respectively. This clearly shows that the holey AAs-gC3N4 nanosheets interacted synergistically with the NiTiO3 NFs. This extended the lifetime of photogenerated charge carriers and resulted in superior photocatalytic activity compared with pristine NiTiO3 NFs and bulk gC3N4. The higher Brunauer-Emmett-Teller surface area and the presence of many catalytically active sites also enhanced the photocatalytic performance of the hybrid sample. Moreover, through photoluminescence and photocurrent response analysis, a significant decrease in the recombination losses of the hybrid photocatalysts was also confirmed. Thus, this is a novel strategy to fabricate highly efficient photocatalysts with precisely tunable operating windows and enhanced charge separation.
Herein, a full spectrum-induced hybrid structure consisting of one-dimensional nickel titanate (NiTiO3) nanofibers (NFs) decorated by petal-like molybdenum disulfide (MoS2) particles was designed through a facile hydrothermal method. The key parameters for tailoring the morphology and chemical, surface, and interfacial properties of the heterostructure were identified for efficient and selective conversion of CO2 into valuable chemicals. Introducing MoS2 layers onto NiTiO3 NFs provided superior CO2 conversion with significantly higher yields. The optimized hybrid structure produced CO and CH4 yields of 130 and 55 μmol g−1 h−1, respectively, which are 3.8- and 3.6-times higher than those from pristine NiTiO3 nanofibers (34 and 15 μmol g−1 h−1, respectively) and 3.6- and 5.5-times higher than those from pristine MoS2 (37 and 10 μmol g−1 h−1, respectively). This improved performance was attributed to efficient absorption of a wider spectrum of light and efficient transfer of electrons across the heterojunction. Effective charge separation and reduced charge carrier recombination were confirmed by photoluminescence and impedance measurements. The performance may also be partly due to enhanced hydrophobicity of the hierarchical surfaces due to MoS2 growth. This strategy contributes to the rational design of perovskite-based photocatalysts for CO2 reduction.
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