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Photocatalytic propylene epoxidation with O2 over 4,4′-dibromobenzophenone modified carbon nitride coupled with TS-1

Journal 2024 · IF 8.1 · 发表于 2024 年 2 月 19 日
作者: Haonan Zhang,Changhe Lu,Shuai Wang,Qinhua Zhang,Qiang Zhou,Shuxu Zhu,Chong Qi,Mingbo Wu,Wenting Wu
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摘要

The utilization of O 2 for propylene epoxidation is a highly desirable reaction due to its 100 % atom economy. However, achieving this reaction under mild conditions presents a significant challenge. In this paper, we present a tandem reaction system that combines 4,4′-dibromobenzophenone (BP) modified carbon nitride (g-C 3 N 4 ) with titanium silicalite zeolite (TS-1) to enable the selective photooxidation of propylene into propylene oxide at room temperature, using O 2 as the oxygen source. The achieved production rate of propylene oxide was an impressive 1195 μmol/g cat. /h, with a selectivity exceeding 99 %. Furthermore, the catalyst exhibited no significant deactivation after 5 cycles. Spectra and in-situ capture experiments revealed that the reaction involved a two-step system, with photocatalytic production of H 2 O 2 and propylene epoxidation facilitated by H 2 O 2 ·H 2 O 2 was generated through O 2− and 1 O 2 pathways, with an in-situ utilization efficiency of H 2 O 2 reaching 82 %. This work presents a novel approach for the direct epoxidation of propylene using O 2 .

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