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−1 −1 microproes (0.2 mmol·gcat ·h ). The FE towards ethanol generation could be maintained at a high value of 78% at −0.56 V vs. RHE. In another exciting example, boron and nitrogen co-doped nanodimond was reported for selective reduction of CO2 to ethanol with a maximum FE of 93.2% at −1.0 V vs. RHE in 0.1 M NaHCO3 [83]. The synegic effect of boron and nitrogen codoping and fine balance between nitrogen content and H2 evolution potential drives the highly selective ethanol Catalysts 2020, 10, 1287 15 of 25 formation. These results open new insight into electrochemical conversion of CO2 to clean fuel ethanol. Figure 7. (A) Illustration of cylindrical mesoporous nitrogen-doped carbon (c-NC) and the inverse Figure 7. (A) Illustration of cylindrical mesoporous nitrogen-doped carbon (c-NC) and the inverse mesoporous N-doped carbon (i-NC) for CO2 electroreduction. (B) TEM images of (a1,a2) c-NC and mesoporous N-doped carbon (i-NC) for CO2 electroreduction. (B) TEM images of (a1, a2) c-NC and (b1,b2) i-NC viewed along (a1,b1) (110) and (a2,b2) (100) directions. (C) FEs of CO2 electroreduction products over c-NC and i-NC catalysts at various applied potentials. Reproduced with permission [81]. Copyright 2017, Wiley. 3.2. Photocatalytic CO2 Reduction to Ethanol Photocatalytic CO2 reduction has been paid consistent attention for several decades based on the utilization of solar energy and the concept of artificial photosynthesis [92–94]. During the reduction process of CO2, photocatalysts play a key role in lowering the potential of the electron-proton transfer reaction and the eventual catalytic performance. To date, many kinds of semiconductors have been employed as the photocatalysts for CO2 reduction to solar fuels [95,96]. However, very few semiconductors like TiO2 and graphitic carbon nitride (g-C3N4) can photocatalyze the ethanol formation. 3.2.1. TiO2 Actually, TiO2 is considered the most appropriate candidate of photocatalysts due to its comparable conduction band energy (Ecb ≈ −0.5 eV vs. NHE at pH = 7 as shown in Figure 1) to the reduction potentials of CO2 (Reaction (1)–(7) in Table 1). However, it has yielded low CO2 conversion rates to date, and mainly C1 products of methane and methanol. For the sake of improving catalytic activity and producing ethanol, the incorporating strategies with metals, nonmetals and photosensitive materials have been adopted to modify TiO2. For example, Rh and Pd nanowires with high density of grain boundaries were in situ grown on TiO2 nanosheets, acting as the cocatalysts to enhance photocatalytic CO2 reduction performance [97]. The TiO2-Rh long nanowires and TiO2-Pd nanowires composites catalyzed CO2 reduction to ethanol with an average production rate of 12.1 and 13 μmol·−1·h−1, respectively, during the 4 h reaction under UV light (λ < 400 nm). Depositing 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 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]. The photosensitive AgBr with aPDF Image | Advances in Clean Fuel Ethanol Production from CO2 Reduction
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