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Cobalt Single-Atom-Intercalated Molybdenum Disulfide for Sulfide Oxidation with Exceptional Chemoselectivity.
Advanced Materials ( IF 27.4 ) Pub Date : 2019-11-28 , DOI: 10.1002/adma.201906437
Zhongxin Chen 1 , Cuibo Liu 1, 2 , Jia Liu 1 , Jing Li 1 , Shibo Xi 3 , Xiao Chi 1 , Haisen Xu 1 , In-Hyeok Park 1 , Xinwen Peng 4 , Xing Li 1 , Wei Yu 1 , Xiaowang Liu 5 , Linxin Zhong 4 , Kai Leng 1 , Wei Huang 5 , Ming Joo Koh 1 , Kian Ping Loh 1
Affiliation  

The identification of chemoselective oxidation process en route to fine chemicals and specialty chemicals is a long-standing pursuit in chemical synthesis. A vertically structured, cobalt single atom-intercalated molybdenum disulfide catalyst (Co1 -in-MoS2 ) is developed for the chemoselective transformation of sulfides to sulfone derivatives. The single-atom encapsulation alters the electron structure of catalyst owing to confinement effect and strong metal-substrate interaction, thus enhancing adsorption of sulfides and chemoselective oxidation at the edge sites of MoS2 to achieve excellent yields of up to 99% for 34 examples. The synthetic scopes can be extended to sulfide-bearing alkenes, alkynes, aldehydes, ketones, boronic esters, and amines derivatives as a toolbox for the synthesis of high-value, multifunctional sulfones and late-stage functionalization of pharmaceuticals, e.g., Tamiflu. The synthetic utility of cobalt single atom-intercalated MoS2 , together with its reusability, scalability, and simplified purification process, renders it promising for industrial productions.

中文翻译:

钴单原子嵌入二硫化钼,具有出色的化学选择性,可用于硫化物氧化。

对精细化学品和特种化学品进行化学选择性氧化过程的鉴定是化学合成领域的长期追求。开发了一种垂直结构的钴单原子嵌入的二硫化钼钴催化剂(Co1-in-MoS2),用于将硫化物化学选择性转化为砜衍生物。由于限制作用和强的金属-底物相互作用,单原子包封改变了催化剂的电子结构,从而增强了硫化物在MoS2边缘部位的吸附和化学选择性氧化,从而获得了34个实例的高达99%的优异产率。合成范围可以扩展到含硫化物的烯烃,炔烃,醛,酮,硼酸酯和胺衍生物,作为合成高价值,多功能砜和药物(例如达菲)的后期功能化。钴单原子插层式MoS2的合成用途,以及其可重复使用性,可扩展性和简化的纯化工艺,使其在工业生产中具有广阔的前景。
更新日期:2020-01-27
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