Efficient and Selective C-C Bond Cleavage of a Lignin Model Using a Polyimide Photocatalyst with High Photooxidation Capability

被引:28
|
作者
Wang, Xintie [1 ]
Chu, Sheng [1 ]
Shao, Jingjing [1 ]
Liu, Chao [1 ]
Luo, Zhicheng [1 ]
Xiao, Rui [1 ]
Zhang, Huiyan [1 ]
机构
[1] Southeast Univ, Sch Energy & Environm, Key Lab Energy Thermal Convers & Control, Minist Educ, Nanjing 210096, Peoples R China
来源
ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2022年 / 10卷 / 35期
基金
中国国家自然科学基金;
关键词
lignin; photocatalysis; C-C bond cleavage; polyimide; band structure; GRAPHITIC CARBON NITRIDE; VISIBLE-LIGHT; LIGNOCELLULOSIC BIOMASS; OXIDATION; DEGRADATION; DRIVEN; DEPOLYMERIZATION; VALORIZATION; CHEMICALS; HYDROGENOLYSIS;
D O I
10.1021/acssuschemeng.2c02991
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Lignin represents the most abundant and sustainable aromatic resource to produce value-added aromatics. However, an efficient and selective cleavage of recalcitrant C-C bonds in lignin under mild conditions remains challenging. Photocatalysis has emerged as a promising strategy for such a C-C bond cleavage under ambient conditions, although the activity and selectivity need to be further improved. Herein, using polyimide as a photocatalyst, we report an efficient and selective C-C bond cleavage in a beta-O-4 lignin model under visible light at room temperature. The lignin model was converted into aromatic products with > 99% substrate conversion and > 99% C-C bond cleavage selectivity, which are superior to previously reported photocatalytic systems. Experimental investigations together with theoretical calculations indicated that the superior performance of the polyimide photocatalyst was attributed to its strong photooxidation capability and efficient charge carrier separation efficiency. Mechanistic studies revealed that the dehydrogenation of the lignin model driven by photogenerated holes was the rate-determining step. This work provides useful for the of photocatalysts for selective C-C bond of
引用
收藏
页码:11555 / 11566
页数:12
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