Electrocatalytic Cleavage of C–C Bonds in Lignin Models Using Nonmetallic Catalysts at Ambient Conditions

Guangyong Liu, Ziqi Zhai, Yumiao Lu, JunFeng Lu, Yanlei Wang, Shijing Liang*, Hongyan He* and Lilong Jiang, 
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Abstract

Lignin, characterized by its amorphous, heavily polymerized structure, is a primary natural source of aromatic compounds, yet its complex constitution poses considerable challenges in its transformation and utilization. Therefore, the selective cleavage of C–C bonds represents a critical and challenging step in lignin degradation, essential for the production of high-value aromatic compounds. In this study, we report a simple electrocatalytic approach for lignin valorization via C–C bond cleavage by developing a nonmetallic electrocatalyst of carbon-based materials. It is found that the hydrophilicity and hydrophobicity of the electrocatalyst have a significant effect on the degradation process. Under mild conditions, the hydrophilic carbon paper exhibits 100% substrate conversion, yielding 97% benzaldehyde and 96% quinone with ionic liquid electrolytes. The mechanism study shows that the carbon catalyst with higher surface defects favors electron transfer in the oxidative cleavage process of C–C bonds. These results signify a substantial advancement in lignin degradation, offering an environmentally friendly, metal-free electrochemical route.

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在环境条件下使用非金属催化剂电催化裂解木质素模型中的 C-C 键
木质素具有无定形、高度聚合的结构,是芳香族化合物的主要天然来源,但其复杂的结构给其转化和利用带来了相当大的挑战。因此,C-C 键的选择性裂解是木质素降解过程中具有挑战性的关键步骤,对于生产高价值的芳香族化合物至关重要。在本研究中,我们通过开发碳基材料的非金属电催化剂,报告了一种通过 C-C 键裂解实现木质素价值化的简单电催化方法。研究发现,电催化剂的亲水性和疏水性对降解过程有显著影响。在温和条件下,亲水性碳纸的底物转化率达到 100%,在离子液体电解质的作用下,苯甲醛和醌的产率分别达到 97% 和 96%。机理研究表明,表面缺陷较多的碳催化剂有利于 C-C 键氧化裂解过程中的电子转移。这些结果标志着木质素降解技术取得了重大进展,提供了一种环境友好的无金属电化学途径。
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