Electrocatalytic Lignin Valorization into Aromatic Products via Oxidative Cleavage of C α −C β Bonds

化学 木质素 电催化剂 催化作用 有机溶剂 键裂 电化学 有机化学 电极 物理化学
作者
Jianing Xu,Juan Meng,Yi Hu,Yongzhuang Liu,Yuhan Lou,Wenjing Bai,Shuo Dou,Haipeng Yu,Shuangyin Wang
出处
期刊:Research [American Association for the Advancement of Science]
卷期号:6 被引量:10
标识
DOI:10.34133/research.0288
摘要

Lignin is the most promising candidate for producing aromatic compounds from biomass. However, the challenge lies in the cleavage of C-C bonds between lignin monomers under mild conditions, as these bonds have high dissociation energy. Electrochemical oxidation, which allows for mild cleavage of C-C bonds, is considered an attractive solution. To achieve low-energy consumption in the valorization of lignin, the use of highly efficient electrocatalysts is essential. In this study, a meticulously designed catalyst consisting of cobalt-doped nickel (oxy)hydroxide on molybdenum disulfide heterojunction was developed. The presence of molybdenum in a high valence state promoted the adsorption of tert-butyl hydroperoxide, leading to the formation of critical radical intermediates. In addition, the incorporation of cobalt doping regulated the electronic structure of nickel, resulting in a lower energy barrier. As a result, the heterojunction catalyst demonstrated a selectivity of 85.36% for cleaving the Cα-Cβ bond in lignin model compound, achieving a substrate conversion of 93.69% under ambient conditions. In addition, the electrocatalyst depolymerized 49.82 wt% of soluble fractions from organosolv lignin (OL), resulting in a yield of up to 13 wt% of aromatic monomers. Significantly, the effectiveness of the prepared electrocatalyst was also demonstrated using industrial Kraft lignin (KL). Therefore, this research offers a practical approach for implementing electrocatalytic oxidation in lignin refining.
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