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Molecules 2020, 25, 3653 14 of 23 of its excellent biocompatibility and charge transfer ability [135]. The PDA layer on the electrode can fulfill the requirement of electron transfer and enzyme stabilization and extend the service life of the enzyme [136]. A similar photoelectrochemical cell was constructed by the EC-incorporated PDA bioelectrode and cobalt phosphate/bismuth vanadate (CoPi/BiVO4) photoanode by which the reduction of CO2 can be achieved without external bias. In another study, a voltage was applied to the constructed PEC cell-Co-Pi/Fe2O3 photoanode and BiFeO3 photocathode [137]. The polarization treatment drove surface charge accumulation and accelerated the transfer of electrons to the electrolyte, therefore resulting in an improvement in CO2 conversion efficiency. The tandem PEC cell with an integrated enzyme cascade (TPIEC) system mimics the natural photosynthetic Z-scheme for the biocatalytic reduction of CO2 to methanol. The rate of methanol production per unit of reaction volume and the rate of methanol production per unit mass of photocatalyst can reach 220 μM h−1 and 220 μM gcat−1 h−1, respectively. This device exhibited significantly higher rate of methanol than those of other studies. Due to the relatively high price of the metal rhodium complex [138], researchers further improved the structure of the photoelectrochemical cell to reduce the cost. Neutral red was used as an alternative electron mediator to replace the metal rhodium complex and was conducive to electron recycling between the electrode and NAD+ [139]. Sokol and coauthors [140] adopted a semi-artificial design. The cathode containing formate dehydrogenase was connected to the photoanode containing photosynthetic water oxidase (photosystem II) to achieve the metabolic pathway of formic acid that is formed by light fixation of CO2 in the absence of precious metal catalyst (Figure 9). This demonstrated the feasibility of the nonmetal catalysts for the conversion of CO2 to formic acid and provides a novel method for CO2 photoelectrochemical reduction. Table 3 lists the performance parameters of different photoelectrochemical/enzyme systems. Molecules 2020, 25, x FOR PEER REVIEW 15 of 24 Figure 9. Schematic representation of the semi-artificial photosynthetic tandem PEC cell coupling Figure 9. Schematic representation of the semi-artificial photosynthetic tandem PEC cell coupling CO2 CO2 reduction to water oxidation. A blend of POs and PSII adsorbed on a dpp-sensitized photoanode reduction to water oxidation. A blend of POs and PSII adsorbed on a dpp-sensitized photoanode (IO- (IO-TiO2|dpp|POs-PSII) is wired to an IO-TiO2|FDH cathode [140]. TiO2|dpp|POs-PSII) is wired to an IO-TiO2|FDH cathode [140]. Table 3. Performance comparison of different coupled photoelectrocatalytic/enzymatic CO2 reduction systems. Table 3. Performance comparison of different coupled photoelectrocatalytic/enzymatic CO2 reduction systems. a HCOOH, 6.4 μM h−1 Efficiency Photoanode Photocathode ITO/FDH Photocathode Efficiency Ref. [131] Ref. Co-Pi/Fe O Photoan2od3e a CoPi/BiVO4 Co-Pi/Fe2O3 EC-PDA HCOOH, FE: 99.18% HCOOH, 6.4−1 μM h−1 [112] [131] Co-Pi/αoFe2O3 FTO/ICO-oTPiOi/B/diPVPO/P4 ITO/FDH FTO/IOE-TCiO-P/FDAH FTO/FeOOH/BiVO FTO/3D TiN-ClFDH –2 HCOOH, 0.78 μM h−1, FE: 77.3% BiFeO3-CcFDH/PcFaldDH/YADH CH3OH, 220 μM h HCOHOHC,O0.O18H5 μ,MFEcm: 99.18% [137] [14[01]12] [113] [14[1]37] [142] -PSII 2Os 2 BiFeO3- Co-PTiK/α/ToiOFe2O3 FDH-CHV(CH)COOH HCOOCHH,30O.0HnM,2a2ft0er3μhMh−1 Plain graphite rod FTO/IO-TiO2/dPP/POs- PSII FTO/FeOOH/BiVO4 TK/TiO2 Plain graphite rod CcFDH/PcFaldDH/YADH −1 −1 Pt-FDH HCOOH, 15.49 μM mg Enzyme min 4 2329 a The efficiency includes the product and rates. –2 FTO/IO-TiO2/FDH FTO/3D TiN-ClFDH FDH-CH3V(CH2)9COOH Pt-FDH HCOOH, 0.185 μM cm HCOOH, 0.78 μM h−1, FE: 77.3% HCOOH, 30.0 nM after 3 h HCOOH, 15.49 μM mg Enzyme−1 min−1 [140] [113] [141] [142] a The efficiency includes the product and rates.PDF Image | Research Progress in Conversion of CO2 to Valuable Fuels
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