期刊
CHEMICAL ENGINEERING JOURNAL
卷 452, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.139477
关键词
Biomass conversion; Biofuels; Photocatalysis; Host-guest chemistry; Supramolecular chemistry
The appropriate regulation of photocatalyst band structure by introducing active sites is an effective strategy for constructing efficient photocatalytic systems for biomass valorization. In this study, a renewed host-guest photocatalyst (Ov-WO3@CB[5]) was prepared by anchoring cucurbit[5]uril on oxygen vacancy-rich WO3. It demonstrated efficient reductive upgrading of biomass derivatives and quantitative production of bio-alcohols or arylamines. The inclusion of cucurbit[5]uril adjusted the semiconductor band structure, enhanced carrier migration efficiency, and facilitated the entrance of NH3-BH3, as supported by theoretical calculations.
The appropriate regulation of photocatalyst band structure by simultaneous introduction of active sites is an effective strategy in constructing efficient photocatalytic systems for biomass valorization. Herein, a renewed host-guest photocatalyst (Ov-WO3@CB[5]) prepared by anchoring cucurbit[5]uril on oxygen vacancy-rich WO3 was efficient for reductive upgrading of biomass derivatives using NH3-BH3, such as cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to gamma-valerolactone (up to 99 % yield) at 25 degrees C in 1 h, and quan-titative production of primary/secondary bio-alcohols or arylamines from various aldehydes/ketones or nitro-arenes, respectively. Also, the rate of H2 production by direct photocatalytic hydrolysis of NH3-BH3 could reach 5.75 mL h-1 g-1. The inclusion of cucurbit[5]uril effectively adjusted the semiconductor band structure and enhanced migration efficiency of photo-generated carriers, and the hydrophobic cavity of cucurbit[5]uril favored the entrance of NH3-BH3, as elaborated by theoretical calculations. Properly engineering supramolecular surface-active sites based on interface host-guest chemistry opens new avenues for reductive upgrading of biomass and hydrogen evolution.
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