化学
催化作用
硫化物
光化学
化学工程
光催化
选择性
可见光谱
激子
纳米技术
材料科学
有机化学
光电子学
量子力学
物理
工程类
作者
Jingjun Li,Yanning Chen,Xue Yang,Shuiying Gao,Rong Cao
标识
DOI:10.1016/j.jcat.2019.11.041
摘要
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.
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