Publication date: 10th October 2023
CdS quantum dots (QDs), acting as photosensitizers, or sometimes solo photocatalysts in CO2 reduction, have offered a myriad of advantages including quantum confinement effect, surface functionalization, tunable redox potential, and photoreduction selectivity. However, CdS QDs are frequently compromised by thermal and oxidative instability, as well as photocorrosion, which restricts their practical applications. We propose an effective method endowing CdS QDs by assembling with amphiphilic metallopolymer (Re-IL) to enhance their stability and synergistic activity. The thioglycolic acid-capped cadmium sulfide quantum dots (TGA-CdS CdS) were successfully prepared using a simple reflux method. The amphiphilic metallopolymers were synthesized via precise radical polymerization between 1-ethyl-3-vinylimidazolium bromide and 1-50 mol% of a literature new rhenium(I)-N-(3-((4'-methoxy-[2,2'-bipyridin]-4-yl)oxy)propyl)-acrylamide compounds. Electrostatic interaction facilitated the spontaneous self-assembly of Re-IL onto TGA-CdS QDs facilitating photo-induced electron transfer (PET) from TGA-CdS QDs to vicinal bipyridyl ReI(CO)3Cl derivatives in water and a mixture of DMF/water. All hybrid catalysts (Re-IL/TGA-CdS QDs) demonstrated synergistically boosting photocatalytic CO2 reduction to yield CO with over 90% selectivity in 25 mL DMF/water (4:1 v/v), under LED 370 nm irradiation. This research also sheds light on rational designs of hybrid catalytic materials for high CO2 reduction performance, selectivity, and stability in the future.
This work was supported by the Thailand Science Research and Innovation Fund Chulalongkorn University, the Thailand Toray Science Foundation (Science and Technology Research Grants 2021), the National Research Council of Thailand (NRCT), Office of the Ministry of Higher Education, Science, Research and Innovation, and the Development and Promotion of Science and Technology Talents Project (DPST).
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