Journal
ACS CATALYSIS
Volume 9, Issue 3, Pages 2580-2593Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b03816
Keywords
CO2 to formate conversion; organic-inorganic hybrid systems; molecular catalyst TiO2 immobilization; heterogeneous catalysis; photocatalysis
Categories
Funding
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2014R1A6A1030732, NRF-2016R1D1A3B03934670, NRF-2016R1D1A3B03936414]
- Functional Districts of the Science Belt support program, Ministry of Science, ICT and Future Planning [2015K000287]
- Next Generation Carbon Upcycling Project of Climate Change Response Project - MSIT of Republic of Korea [NRF-2017M1A2A2046738]
- KOREA RESEARCH INSTITUTE of CHEMICAL TECHNOLOGY (KRICT)
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A Mn(I)-based hybrid system (OrgD-vertical bar TiO2 vertical bar-MnP) for photocatalytic CO2 reduction is designed to be a coassembly of Mn(4,4'-Y-2-bpy)(CO)(3)Br (MnP; Y = CH2PO (OH)(2)) and (E)-3-[5-(4-(diphenylamino)phenyl)-2,2'-bithiophen-2'-y1]-2-cyanoacrylic acid (OrgD) on TiO2 semiconductor particles. The OrgD-vertical bar TiO2 vertical bar-MnP hybrid reveals persistent photocatalytic behavior, giving high turnover numbers and good product selectivity (HCOO- versus CO). As a typical run, visible-light irradiation of the hybrid catalyst in the presence of 0.1 M electron donor (ED) and 0.001 M LiCIO4 persistently produced HCOO- with a >99% selectivity accompanied by a trace amount of CO; the turnover number (TONformate) reached,similar to 250 after 23 h of irradiation. The product selectivity (HCOO-/CO) was found to be controlled by changing the loading amount of MnP on the TiO2 surface. In situ FTIR analysis of the hybrid during photocatalysis revealed that, at low Mn concentration, the Mn-H monomeric mechanism associated with HCOO- formation is dominant, whereas at high Mn concentration, CO is formed via a Mn-Mn dimer mechanism.
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