The Crucial Role of Oxygen Evolution Reaction in Electrocatalytic Oxidative C─C Bond Cleavage in Lignin Biomass Valorization

J Jingxuan Zhang W Wenjing Bai J Jianing Xu (Program in Molecular Pharmacology, Department of Medicine, Memorial Sloan Kettering Cancer Center) A Ao Zhou J Jialin Fan (State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China) J Junlu Bi (State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China) Q Qingguo Zhou (State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China) L Liyuan Gong (State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University Changsha 410082 China) Y Yongzhuang Liu (State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China) S Shuo Dou (State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China) H Haipeng Yu (State Key Laboratory of Microbial Technology, Institute of Microbial Technology) S Shuangyin Wang (State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering)

Abstract

Abstract The electrocatalytic oxidative cleavage of the C─C bond is highly effective for converting lignin biomass into high‐value‐added aromatic chemicals. However, the oxygen evolution reaction (OER) at applied oxidative potential usually competes in the aqueous environment. In this study, we found that OER does not entirely hinder the cleavage process but rather acts as a synergistic catalytic step. By using defect‐rich carbon nanotubes as the electrocatalyst and combining experimental and theoretical analysis, we found that the reactive oxygen species (O 2 − ) formed before *O 2 desorption serve as the key oxygen source. These species could interact with the enolate intermediate of lignin, which facilitates the in situ production of aromatic compounds. Under the optimal potential of 0.5 V versus Ag/AgCl, 98.8% of 2‐phenoxyacetophenone is converted into phenol and benzoic acid via C α ─C β bond cleavage, with yields of 62.31% and 43.42%, respectively. Additionally, the depolymerization of quasi‐natural poplar lignin achieves a total monomer yield of up to 12.41 wt%. This study provides new mechanistic insights into C α ─C β bond cleavage during electrocatalytic lignin depolymerization under alkaline conditions, contributing to efficient biomass valorization.

Article Details

Volume / Issue Vol. 64, Issue 32
Published August 04, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (12)

J

Jingxuan Zhang

W

Wenjing Bai

J

Jianing Xu

Program in Molecular Pharmacology, Department of Medicine, Memorial Sloan Kettering Cancer Center

A

Ao Zhou

J

Jialin Fan

State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China

J

Junlu Bi

State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China

Q

Qingguo Zhou

State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China

L

Liyuan Gong

State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University Changsha 410082 China

Y

Yongzhuang Liu

State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China

S

Shuo Dou

State Key Laboratory of Utilization of Woody Oil Resource, Key Laboratory of Bio‐Based Material Science and Technology of Ministry of Education Northeast Forestry University Harbin 150040 China

H

Haipeng Yu

State Key Laboratory of Microbial Technology, Institute of Microbial Technology

S

Shuangyin Wang

State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering