Proceedings of Catalyst Design Strategies for Photo- and Electrochemical Fuel Synthesis (ECAT25)
Publication date: 19th December 2024
Photocatalysts can convert CO2 to useful products such as formic acid and carbon monoxide using visible light. However, most photocatalysts are limited by impractical stability and low conversion rates.
Conjugated polymers have emerged as promising visible-light-active photocatalysts for solar fuel production due to their ease of optoelectronic tuneability and extensive building block scope to name but a few. Similarly, molecular photocatalysts based on metal complexes have been well studied for photocatalytic CO2 reduction to useful products.
By assembling hybrid photocatalysts[1] consisting of conjugated polymers and a binuclear ruthenium(II)-ruthenium(II) complex, very active photocatalysts were discovered for the conversion of CO2 to formate with augmented activity compared to previously reported literature. The best system produced a turnover number of 349,000 (one-order higher than the previously reported most durable system),[2] a turnover frequency of 6.5 s-1 (surpassing that of CO2 fixation by RuBisCO in natural photosynthesis, ~3 s‑1),[3] and an apparent quantum yield of 11.2% at 440 nm (the highest amongst hybrid photocatalysts reported to date).[4]
Remarkably, quantitative conversion of CO2 to formate was achieved at standard conditions, thereby enabling the use of low concentration CO2 feedstocks (especially flue gas streams which are ~3-13% CO2 by composition) which is very relevant for practical application. After full consumption of CO2, further replenishment with more CO2 feedstock produced a very high concentration of formate up to 0.40 M within the timeframe studied and without significant decomposition of the photocatalyst. The use of transient absorption spectroscopy allowed insightful elucidation of the key structure-activity factors which led to the remarkably high photocatalytic activity in the most active system.
This direct light-driven conversion of CO2 to highly concentrated formate offers a more sustainable alternative than current feedstocks by enabling a carbon neutral pathway mediated by solar energy in the supply chain.
Thanks is given to the EPSRC for funding through a Doctoral Training Partnership postgraduate studentship (EP/T517938/1) and the EPSRC Supergen Solar Network+ (EP/S000763/1).
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