Highly selective oxidation of benzene to phenol with air at room temperature promoted by water

被引:38
作者
Xie, Jijia [1 ,8 ]
Li, Xiyi [1 ]
Guo, Jian [2 ,9 ]
Luo, Lei [3 ,10 ]
Delgado, Juan J. [4 ,5 ]
Martsinovich, Natalia [6 ]
Tang, Junwang [1 ,7 ]
机构
[1] UCL, Dept Chem Engn, London WC1E 7JE, England
[2] UCL, Dept Chem, London WC1H 0AJ, England
[3] Northwest Univ, Coll Chem & Mat Sci, Key Lab Synthet & Nat Funct, Mol Chem Minist Educ, Xian 710127, Peoples R China
[4] Univ Cadiz, Fac Ciencias, Dept Ciencia Mat Ingn Metalurg & Quim Inorgan, Campus Rio San Pedro, Cadiz 11510, Spain
[5] Inst Microscopia Elect & Mat, IMEYMAT, Puerto Real 11510, Spain
[6] Univ Sheffield, Dept Chem, Sheffield S3 7HF, England
[7] Tsinghua Univ, Ind Catalysis Ctr, Dept Chem Engn, Beijing 100084, Peoples R China
[8] Sinopec Beijing Res Inst Chem Ind, Sinopec Grp, Beijing 100013, Peoples R China
[9] Sichuan Univ, Coll Phys, Chengdu 610064, Sichuan, Peoples R China
[10] Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat iChEM, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China
基金
英国工程与自然科学研究理事会; 中国博士后科学基金;
关键词
HYDROGEN-PRODUCTION; RUTILE TIO2; HYDROXYLATION; PD; CONVERSION; METHANE; PHOTOCATALYST; MECHANISM; EVOLUTION; PEROXIDE;
D O I
10.1038/s41467-023-40160-w
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Phenol is one of the most important fine chemical intermediates in the synthesis of plastics and drugs with a market size of ca. $30b1 and the commercial production is via a two-step selective oxidation of benzene, requiring high energy input (high temperature and high pressure) in the presence of a corrosive acidic medium, and causing serious environmental issues2-5. Here we present a four-phase interface strategy with well-designed Pd@Cu nanoarchitecture decorated TiO2 as a catalyst in a suspension system. The optimised catalyst leads to a turnover number of 16,000-100,000 for phenol generation with respect to the active sites and an excellent selectivity of ca. 93%. Such unprecedented results are attributed to the efficient activation of benzene by the atomically Cu coated Pd nanoarchitecture, enhanced charge separation, and an oxidant-lean environment. The rational design of catalyst and reaction system provides a green pathway for the selective conversion of symmetric organic molecules. Phenol is one of the most important fine chemicals, but its synthesis is highly energy intensive. Here, the authors report an economical pathway for the selective photocatalytic conversion of benzene to phenol in high yield and selectivity by Pd@Cu/TiO2 catalyst using with air as oxidant.
引用
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页数:12
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