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Visible-light-mediated high-efficiency catalytic oxidation of sulfides using wrinkled C3N4 nanosheets
Journal of Catalysis ( IF 7.3 ) Pub Date : 2019-12-18 , DOI: 10.1016/j.jcat.2019.11.041
Jingjun Li , Yanning Chen , Xue Yang , Shuiying Gao , Rong Cao

Incorporating visible light into sulfide oxidation is an emerging desirable strategy to produce versatile sulfoxides. We introduce the design and synthesis of multilayered wrinkled C3N4 nanosheets and demonstrate their unprecedented sulfide oxidation activity. Due to the wrinkled surfaces with a large SBET (208.6 m2g−1), wrinkled C3N4 nanosheets exhibit a sensitive optical response, facilitating the electron photoexcition. Layer structure confinement enables robust e-h+ interactions and valid photoexcited excitons formation, allowing rapid 1O2 reactive species production. Integrating the sensitive optical response with robust e-h+ interactions, photoexcited electrons and excitons are jointly produced, giving large yields of ⋅O2 and 1O2 reactive species that are conductive to O2 and 1O2 cocatalysis with an activity that is up to 33-fold that of bulk C3N4. In the cocatalysis mechanism, both O2 and 1O2, can produce peroxysulfoxide intermediates, resulting in target sulfoxides. This is the first report on sulfide oxidation via O2 and 1O2 cocatalysis and a promising study on catalyst exploitation for high-efficiency and high-selectivity production process.



中文翻译:

使用皱纹的C 3 N 4纳米片的可见光介导的硫化物的高效催化氧化

将可见光结合到硫化物氧化中是生产通用亚砜的一种新兴的理想策略。我们介绍了多层起皱的C 3 N 4纳米片的设计与合成,并展示了其前所未有的硫化物氧化活性。由于具有大的S BET(208.6 m 2 g -1)的起皱表面,起皱的C 3 N 4纳米片表现出灵敏的光学响应,从而促进了电子的光解吸。层结构限制使鲁棒的e -- h +相互作用和有效的光激发激子形成,可快速产生1 O 2。反应物种的生产。积分用强大的电子敏感的光学响应- -h +相互作用,光激发电子和激子共同制作,得到⋅O的大产率2 -1个ö 2是导电的以反应性物种ö 2 -1 ö 2助催化作用与活性高达C 3 N 4的33倍。在助催化作用机理,二者ö 2 -1 Ò 2,可产生过氧亚砜中间体,产生目标亚砜。这是通过在硫化物氧化的第一份报告Ò 2 -1 Ò 2助催化作用和用于高效率和高选择性生产过程对催化剂开发有希望的研究。

更新日期:2019-12-19
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