Construction of a Cu@hollow TS-1 nanoreactor based on a hierarchical full-spectrum solar light utilization strategy for photothermal synergistic artificial photosynthesis

The artificial photosynthesis technology has been recognized as a promising solution for CO2 utilization. Photothermal catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosynthesis by coupling both photochemistry and thermochemistry. However, strategies for maximizing the use of solar spectra with different frequencies in photothermal catalysis are urgently needed. Here, a hierarchical full-spectrum solar light utilization strategy is proposed. Based on this strategy, a Cu@hollow titanium silicalite-1 zeolite (TS-1) nanoreactor with spatially separated photo/thermal catalytic sites is designed to realize high-efficiency photothermal catalytic artificial photosynthesis. The space-time yield of alcohol products over the optimal catalyst reached 64.4 mu mol g-1 h-1, with the selectivity of CH3CH2OH of 69.5%. This rationally designed hierarchical utilization strategy for solar light can be summarized as follows: (1) high-energy ultraviolet light is utilized to drive the initial and difficult CO2 activation step on the TS-1 shell; (2) visible light can induce the localized surface plasmon resonance effect on plasmonic Cu to generate hot electrons for H2O dissociation and subsequent reaction steps; and (3) low-energy near-infrared light is converted into heat by the simulated greenhouse effect by cavities to accelerate the carrier dynamics. This work provides some scientific and experimental bases for research on novel, highly efficient photothermal catalysts for artificial photosynthesis. A full-spectrum utilization strategy has been proposed to maximize the use of solar light with different frequencies. Based on this strategy, a Cu@hollow-titanium silicalite-1 zeolite nanoreactor is rationally designed to realize enhanced photothermal catalytic performance in artificial photosynthesis. High yield of alcohol products and high selectivity of ethanol can be achieved using an optimal catalyst. image