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Molecules 2020, 25, 3653 7 of 23 Molecules 2020, 25, x FOR PEER REVIEW 7 of 24 Figure 4. Schematic illustration of the structures of M-PMOFs (M = Co, Fe, Ni, Zn). M-TCPP: tetrakis Figure 4. Schematic illustration of the structures of M-PMOFs (M = Co, Fe, Ni, Zn). M-TCPP: tetrakis [4-carboxyphenyl]-porphyrin-M (M-TCPP) linkers [76]. [4-carboxyphenyl]-porphyrin-M (M-TCPP) linkers [76]. to CO on an iron–porphyrin center using a computational modeling. The results showed that a ligand, rather than metal reduction, Davethu et al. [77] studied the electrochemical reduction of CO Davethu et al. [77] studied the electrochemical reduction of CO2 to CO on an iron–porphyrin 2 III 2− − 2− resultedinstablebindingofCO asan[Fe II(ICO 2−)(TPP−)]2− complexduringthereductionprocess. center using a computational modeling. The results showed that a ligand, rather than metal reduction, resulted in stable binding of CO2 as an [ Fe (CO2 ) (TPP )] complex during the reduction process. 22 Subsequent proton transfer from phenol was considered as a proton-coupled electron-transfer process, Subsequent proton transfer from phenol was considered as a proton-coupled electron-transfer and the second proton transfer does not change the electronic configuration of the metal complex. process, and the second proton transfer does not change the electronic configuration of the metal It was demonstrated that iron porphyrin was an effective catalyst and could efficiently transform complex. It was demonstrated that iron porphyrin was an effective catalyst and could efficiently CO toCO.Inaddition,theresultsindicatedthatCO bindingwastherate-determiningstepinthe 22 transform CO2 to CO. In addition, the results indicated that CO2 binding was the rate-determining reaction cycle, providing a promising direction for further optimization. A series of skeletons based on step in the reaction cycle, providing a promising direction for further optimization. A series of porous metal–porphyrin triazine were synthesized by trimming porphyrin units under ionothermal skeletons based on porous metal–porphyrin triazine were synthesized by trimming porphyrin units conditions [78]. The skeletons have high specific surface areas and homogenously dispersed transition under ionothermal conditions [78]. The skeletons have high specific surface areas and homogenously metals.ThisfacilitatestheadsorptionofCO moleculesandexposureoflargernumberofactivesites, 2 dispersed transition metals. This facilitates the adsorption of CO2 molecules and exposure of larger therebyimprovingtheperformanceofCO reduction. number of active sites, thereby improving the performance of CO2 reduction. 2 is, energetically, an uphill process. Many effective and selective homogeneous Reducing CO2 is, energetically, an uphill process. Many effective and selective homogeneous Reducing CO 2 metalcomplexcatalystshavebeendevelopedtopromoteCO conversion.Forexample,anumber 2 metal complex catalysts have been developed to promote CO2 conversion. For example, a number of of pincer complexes can reduce CO into CO, CH , or other compounds [79–82]. The ruthenium 24 pincer complexes can reduce CO2 into CO, CH4, or other compounds [79–82]. The ruthenium catalysts catalysts prepared by different methods are usually used in such systems [83–86] in which the turnover prepared by different methods are usually used in such systems [83–86] in which the turnover number(TON)ofCO tomethanolreached9900atanoptimalcondition.Allofthisshowsthegood 2 number (TON) of CO2 to methanol reached 9900 at an optimal condition. All of this shows the good conductivity and catalytic performance of pincer complexes, but these catalysts often rely on precious conductivity and catalytic performance of pincer complexes, but these catalysts often rely on precious metals or supported ligands, such as bipyridines. Most catalysts used in CO reduction have the 2 metals or supported ligands, such as bipyridines. Most catalysts used in CO2 reduction have the ability of hydrogen evolution, resulting in H generation during the conversion of CO . This will 22 ability of hydrogen evolution, resulting in H2 generation during the conversion of CO2. This will suppress the formation of the desired products because of competition in electron capturing with suppress the formation of the desired products because of competition in electron capturing with the evolution reaction. It is difficult to find a suitable electrocatalyst to selectively improve the H2 evolution reaction. It is difficult to find a suitable electrocatalyst to selectively improve the the H 2 conversionefficiencyofCO [87].Furthermore,multi-electrontransferprocessandelectrontransfer 2 conversion efficiency of CO2 [87]. Furthermore, multi-electron transfer process and electron transfer rate are the critical limiting factors in the electrocatalytic reaction. The main challenge is to find a rate are the critical limiting factors in the electrocatalytic reaction. The main challenge is to find a highly selective electrocatalyst with high catalytic activity and long-term stability to overcome the highly selective electrocatalyst with high catalytic activity and long-term stability to overcome the thermodynamicstabilityofCO molecules.Ifelectrocatalysisandphotocatalysisarecombinedtotake 2 thermodynamic stability of CO2 molecules. If electrocatalysis and photocatalysis are combined to take full advantage of their respective advantages, seem to be a better method to reduce CO . full advantage of their respective advantages, seem to be a better method to reduce CO2. 2PDF Image | Research Progress in Conversion of CO2 to Valuable Fuels
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