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Ni(OH)2 nanosheets onto TiO2 nanofibers could enhance charge separation efficiency and CO2 capture capacity [98]. With 15 wt% Ni(OH)2 loaded, 0.37 μmol·g-1·h-1 of ethanol was achieved over TiO2/Ni(OH)2 hybrid catalyst. In another case, the incorporation of matrix facilitated the effective charge separation and CO2 reduction, in which the average production rate of ethanol was maximized to 13.2 μmol·g−1·h−1 on 1.5wt%Ni2+-TiO2 during 4 h of UV light irradiation [99]. Graphene Catalysts 2020, 10, 1287 16 of 25 quantum dots (GQDs) were combined with vanadium-doped TiO2 (V-TiO2) to effectively separate photogenerated electrons and holes, and 5%GQDs/V-TiO2 exhibited the best photocatalytic activity with an ethanol production rate of 5.65 μmol g−1 h−1 under solar spectrum irradiation (Figure 8) [100]. narrow band gap was coupled with TiO2 to improve the visible light activity, and the 23.2% AgBr/TiO2 The photosensitive AgBr with a narrow band gap was coupled w−i1th −T1iO2 to improve the visible light composite showed a relatively high ethanol yield of 13.28 μmol g h under visible-light irradiation activity, and the 23.2% AgBr/TiO2 composite showed a relatively high ethanol yield of 13.28 μmol g−1 for 5 h [101]. h−1 under visible-light irradiation for 5 h [101]. Figure 8. (A) HRTEM image of 5%GQDs/V-TiO2. The yields of methanol, ethanol and methane (B) under solar spectrum irradiation and (C) under visible light irradiation (λ ≥ 420 nm) on GQDs/V-TiO2 catalysts with different GQD contents. Reproduced with permission [100]. Copyright 2016, American Chemical Society. 3.2.2. G-C3N4 As a novel nonmetallic semiconductor, g-C3N4 with a moderate band gap (Eg = 2.7 eV, as shown in Figure 1) has attracted significant attention in photocatalytic CO2 reduction due to its high stability and responsiveness to visible light. It can be synthesized through the pyrolysis of some nitrogen-rich organic precursors, such as urea and melamine. The g-C3N4 derived from urea (u-g-C3N4) possessed a mesoporous flake-like structure with a larger surface area and photocatalyzed CO2 reduction to ethanol in a yield of 4.5 μmol·g−1·h−1 with methanol as a co-product under visible-light irradiation for 12 h (Figure 9) [102], while the g-C3N4 derived from melamine (m-g-C3N4) without porous structure could exclusively yield ethanol at a lower rate of 3.6 μmol·g−1·h−1. The above-mentioned different photocatalytic activities and selectivities for the formation of ethanol are possibly due to the differences in the crystallinity and microstructure of u-g-C3N4 and m-g-C3N4. The non-porous structure of m-g-C3N4 may not favor the fast exchange of the formed *OCH3 or CH3OH, thus probably promoting the dimerization of *OCH3 to form ethanol. Moreover, much effort has been devoted to improving the photocatalytic activity of g-C3N4 via the combination with other semiconductors. For example, ZnO with a negative conduction band potential of −0.44 eV was coupled with g-C3N4 by an impregnation method to generate ZnO/g-C3N4 composite photocatalyst [103]. Although the CO2 conversion rate was considerably enhanced over the optimal ZnO/g-C3N4 composite, the ethanol yield was still as low as 1.5 μmol·g−1·h−1 under simulated sunlight irradiation. Meanwhile, the Ag3PO4/g-C3N4 composite photocatalyst was also reported to significantly improve the CO2 conversion rate, but exhibit a low ethanol yield of 1.3 μmol·g−1·h−1 under simulated sunlight irradiation [104]. When the two-dimensional g-C3N4 nanosheets with few-layer thickness were used as the support of Pd to ensure equivalent charge migrations to various Pd facets, the selectivity of CO2 photoreduction to ethanol strongly depends on the shapes of Pd nanocrystals on the C3N4 nanosheets [105]. The optimal ethanol production rate was achieved on Pd nanotetrahedrons loaded on g-C3N4 nanosheets with a Pd loading of 5.8 wt%, though the value only arrived at 2.18 μmol·g−1·h−1. Therefore, it still remains challenging to selectively photocatalyze CO2 reduction to ethanol over g-C3N4.PDF Image | Advances in Clean Fuel Ethanol Production from CO2 Reduction
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