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

作　　者：Sixian Zhu Qiao Zhao Hongxia Guo Li Liu Xiao Wang Xiwei Qi Xianguang Meng Wenquan Cui 

机构地区：[1]Hebei Key Laboratory for Environment Photocatalytic and Electrocatalytic Materials,College of Chemical Engineering,North China University of Science and Technology,Tangshan,China [2]School of Materials Science and Engineering,National Institute for Advanced Materials,TKL of Metal and Molecule-Based Material Chemistry,Nankai University,Tianjin,China [3]Hebei Iron and Steel Laboratory,Tangshan,China

出　　处：《Carbon Energy》2024年第2期25-36,共12页碳能源（英文）

基　　金：supported by the National Natural Science Foundation of China(Grant Nos.21908052 and 22108200);the Key Program of the Natural Science Foundation of Hebei Province(Grant No.B2020209017);the Project of Science and Technology Innovation Team,Tangshan(Grant No.20130203D);the Natural Science Foundation of Zhejiang Province(Grant No.LQ22B060013);and the Science and Technology Project of Hebei Education Department(Grant No.QN2021113).

摘　　要：The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) 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 64.4μmol 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 CO_(2) 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.

关 键 词：artificial photosynthesis full spectrum NANOREACTORS photothermal catalysis 

分 类 号：O64[理学—物理化学]