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

Jijia Xie; Xiyi Li; Jian Guo; Lei Luo; Juan J Delgado; Natalia Martsinovich; Junwang Tang

doi:10.1038/s41467-023-40160-w

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

Nat Commun. 2023 Jul 22;14(1):4431. doi: 10.1038/s41467-023-40160-w.

Authors

Jijia Xie^{1

2}, Xiyi Li¹, Jian Guo^{3

4}, Lei Luo^{5

6}, Juan J Delgado^{7

8}, Natalia Martsinovich⁹, Junwang Tang^{10

11}

Affiliations

¹ Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
² Sinopec Beijing Research Institute of Chemical Industry, Sinopec Group, Beijing, 100013, China.
³ Department of Chemistry, University College London, London, WC1H 0AJ, UK.
⁴ College of Physics, Sichuan University, Chengdu, Sichuan, 610064, China.
⁵ Key Lab of Synthetic and Natural Functional, Molecule Chemistry of Ministry of Education, the Energy and Catalysis Hub, College of Chemistry and Materials Science, Northwest University, Xi'an, 710127, China.
⁶ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, The Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Dalian, Liaoning, 116023, China.
⁷ Departamento de Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Rio San Pedro, 11510, Puerto Real, Cádiz, Spain.
⁸ IMEYMAT, Instituto de Microscopía Electrónica y Materiales, Puerto Real, 11510, Spain.
⁹ Department of Chemistry, University of Sheffield, Sheffield, S3 7HF, UK.
¹⁰ Department of Chemical Engineering, University College London, London, WC1E 7JE, UK. junwang.tang@ucl.ac.uk.
¹¹ Industrial Catalysis Center, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China. junwang.tang@ucl.ac.uk.

Abstract

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 issues^2-5. 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.

Abstract

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