Selective Hydrogenation of Phenols to Cyclohexanones Over Hydrotalcite-Supported Pd Single-Atom Catalyst

Yani Liu; Qinglei Meng; Kaili Zhang; Wanying Han; Xinrui Zheng; Yaqin Wang; Yibo Han; Jingping Wang; Haihong Wu; Mingyuan He; Buxing Han

doi:10.1002/anie.202504260

Selective Hydrogenation of Phenols to Cyclohexanones Over Hydrotalcite-Supported Pd Single-Atom Catalyst

Angew Chem Int Ed Engl. 2025 May 19:e202504260. doi: 10.1002/anie.202504260. Online ahead of print.

Authors

Yani Liu^{1

2}, Qinglei Meng³, Kaili Zhang⁴, Wanying Han^{1

2}, Xinrui Zheng^{1

2}, Yaqin Wang^{1

2}, Yibo Han^{1

2}, Jingping Wang^{1

2}, Haihong Wu^{1

2}, Mingyuan He^{1

2}, Buxing Han^{1

2

3}

Affiliations

¹ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.
² Institute of Eco-Chongming, 20 Cuiniao Road, Chenjia Town, Chongming District, Shanghai, 202162, China.
³ Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
⁴ Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, China.

PMID: 40388558
DOI: 10.1002/anie.202504260

Abstract

Cyclohexanones are widely used chemicals and currently produced by the oxidation of the fossil feedstocks. Direct selective hydrogenation of lignin derivatives has great potential for producing these chemicals, but is challenging to obtain high yields. Here, we report that hydrotalcite-supported Pd single-atom (Pd/CHT-800) catalyst enabled the hydrogenation of the benzene ring in the aromatics without the overreaction of carbonyl group, which could afford >99.9% yield of cyclohexanones using water as the reaction medium. The reaction mechanism was systematically studied by the control experiments and detailed in situ characterizations. In the Pd/CHT-800 catalyst, the Pd-O-MgAl sites were formed, and the cooperation of the Pd atoms and calcined CHT material could not only realize the aromatic hydrogenation efficiently, but also inhibit the hydrogenation of the carbonyl group in the reaction effectively. This work provides a novel route for the sustainable production of cyclohexanones.

Keywords: Aromatics; Cyclohexanones; Hydrogenation; Single‐atom catalyst.

Abstract

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