Photothermal catalytic transfer hydrogenolysis of protolignin

Hongji Li; Xiaotong Sun; Ting Li; Zhitong Zhao; Hui Wang; Xiaomei Yang; Chaofeng Zhang; Feng Wang

doi:10.1038/s41467-024-54664-6

Photothermal catalytic transfer hydrogenolysis of protolignin

Nat Commun. 2024 Nov 23;15(1):10176. doi: 10.1038/s41467-024-54664-6.

Authors

Hongji Li¹, Xiaotong Sun², Ting Li³, Zhitong Zhao⁴, Hui Wang², Xiaomei Yang², Chaofeng Zhang⁵, Feng Wang^{6

7}

Affiliations

¹ College of Chemistry, Zhengzhou University, 100 Science Avenue, Zhengzhou, China. hongjili@zzu.edu.cn.
² College of Chemistry, Zhengzhou University, 100 Science Avenue, Zhengzhou, China.
³ Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Light Industry and Food Engineering, Nanjing Forestry University, 159 LongPan Road, Nanjing, China.
⁴ College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, China.
⁵ Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Light Industry and Food Engineering, Nanjing Forestry University, 159 LongPan Road, Nanjing, China. zhangchaofeng@njfu.edu.cn.
⁶ State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, China. wangfeng@dicp.ac.cn.
⁷ University of Chinese Academy of Sciences, Beijing, China. wangfeng@dicp.ac.cn.

PMID: 39580480
DOI: 10.1038/s41467-024-54664-6

Abstract

Photothermal catalysis is a promising strategy to combine the advantages of both thermal-catalysis and photocatalysis. Herein we achieve the protolignin conversion to aromatics via the photothermal catalytic transfer hydrogenolysis process intensified by the in-situ protection strategy. The Pd/TiO₂ at 140 °C with UV irradiation can catalyze the reforming of primary alcohols to aldehydes and active H* species, which further participate in the acetalation protection of the 1,3-diol group of β-O-4 linkage and mediate the hydrogenolysis of C_β-OAr bonds, respectively. The conversion of birch sawdust with ethanol as the hydrogen donor provides a 40 wt% yield of phenolic monomers, compared with an 11 wt% monomer yield obtained from the conversion of extracted 1,3-diol-protected lignin under the same conditions. The synergistic effect of photocatalysis and thermal-catalysis contributes to the prior cleavage of the C_β-OAr bond before other C-O bonds. The feasibility of solar-light-driven photothermal catalytic system is demonstrated.