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Oxygen-vacancy-assisted construction of Ce–TiO2 aerogel for efficiently boosting photocatalytic CO2 reduction without any sacrifice agent

Journal 2022 · IF 5.532 · 49(4): 6100-6112 · 发表于 2022 年 10 月 17 日
作者: Yu Xia,Jianwei Man,Xiaodong Wu,Shuntian Huang,Anqi Lu,Xiaodong Shen,Sheng Cui,Xiangbao Chen,Gengtao Fu
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摘要

The development of efficient photocatalysts with high activity and high selectivity remains the biggest challenge limiting the development of photocatalysis . Herein, a novel Ce-doped TiO 2 aerogel (Ce–TiO 2 ) is synthesized via a simple one-step sol-gel technique, which integrates simultaneously supercritical drying, heat treatment, nano structuring, and self-diffusion for the formation of the Ce embedded in porous TiO 2 matrix with strong coupling. The Ce–TiO 2 aerogel exhibits typically homogeneous structures, and the resulting Ce–TiO 2 aerogel shows an extremely large BET specific surface area of 246.53 m 2 /g, which is responsible for the much-enhanced photocatalytic active sites. The incorporation of Ce has induced an impurity level in the band gap of the pristine TiO 2 aerogel, extending the light response range to the visible region. Meanwhile, the structural and compositional advantages are exploited to achieve fast separation and transfer of charge carriers. The yields of CH 4 and CO are 0.6 and 2.1 μmol/(g·h) under visible light without any additional co-catalysts or sacrificial agents, which are 1.4 and 15.6 times as high as those of pristine TiO 2 aerogel. In addition, the yields of CH 4 and CO are as high as 10.3 and 26.9 μmol/(g·h) under simulated solar spectrum conditions, which are 34.3 and 1.6 times as high as those of pristine TiO 2 aerogel. The density function theory (DFT) calculation confirms that the resulting Ce–TiO 2 aerogel enables efficient H 2 O and CO 2 adsorption and activation through the Ce cooperation and O vacancy, which greatly improves photocatalytic CO 2 reduction. This work reveals the development of aerogel photocatalyst for the photoreduction of CO 2 with H 2 O and CO 2 as feedstock .