Visible light-driven C-H activation and C-C coupling of methanol into ethylene glycol
Zhang, Qinghong1; Xie, Shunji1; Shen, Zebin1; Deng, Jiao2; Guo, Pu1; Zhang, Haikun1; Ma, Chao3; Jiang, Zheng4; Cheng, Jun1; Deng, Dehui2
刊名NATURE COMMUNICATIONS
2018-03-21
卷号9
ISSN号2041-1723
DOI10.1038/s41467-018-03543-y
文献子类Article
英文摘要The development of new methods for the direct transformation of methanol into two or multi-carbon compounds via controlled carbon-carbon coupling is a highly attractive but challenging goal. Here, we report the first visible-light-driven dehydrogenative coupling of methanol into ethylene glycol, an important chemical currently produced from petroleum. Ethylene glycol is formed with 90% selectivity and high efficiency, together with hydrogen over a molybdenum disulfide nanofoam-modified cadmium sulfide nanorod catalyst. Mechanistic studies reveal a preferential activation of C-H bond instead of O-H bond in methanol by photoexcited holes on CdS via a concerted proton-electron transfer mechanism, forming a hydroxymethyl radical (center dot CH2OH) that can readily desorb from catalyst surfaces for subsequent coupling. This work not only offers an alternative nonpetroleum route for the synthesis of EG but also presents a unique visible-light-driven catalytic C-H activation with the hydroxyl group in the same molecule keeping intact.
WOS关键词HYDROGEN EVOLUTION ; ELECTRON-TRANSFER ; RUTILE TIO2(110) ; WATER ; PHOTOCATALYSIS ; DISSOCIATION ; COCATALYSTS ; CARBON ; BOND
WOS研究方向Science & Technology - Other Topics
语种英语
出版者NATURE PUBLISHING GROUP
WOS记录号WOS:000427929200012
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/168956]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Cheng, Jun; Deng, Dehui; Wang, Ye
作者单位1.Xiamen Univ, Coll Chem & Chem Engn, Natl Engn Lab Green Chem Prod Alcohols Ethers & E, State Key Lab Phys Chem Solid Surfaces,Collaborat, Xiamen 361005, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Collaborat Innovat Ctr Chem Energy Mat, Dalian 116023, Peoples R China
3.Hunan Univ, Coll Mat Sci & Engn, Ctr High Resolut Electron Microscopy, Changsha 410082, Hunan, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
推荐引用方式
GB/T 7714
Zhang, Qinghong,Xie, Shunji,Shen, Zebin,et al. Visible light-driven C-H activation and C-C coupling of methanol into ethylene glycol[J]. NATURE COMMUNICATIONS,2018,9.
APA Zhang, Qinghong.,Xie, Shunji.,Shen, Zebin.,Deng, Jiao.,Guo, Pu.,...&Wang, Ye.(2018).Visible light-driven C-H activation and C-C coupling of methanol into ethylene glycol.NATURE COMMUNICATIONS,9.
MLA Zhang, Qinghong,et al."Visible light-driven C-H activation and C-C coupling of methanol into ethylene glycol".NATURE COMMUNICATIONS 9(2018).
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