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Photocatalytic conversion of lignin into aromatic monomers with adsorbents of radical species from water dissociation
Chem Catalysis ( IF 11.5 ) Pub Date : 2024-07-23 , DOI: 10.1016/j.checat.2024.101066
Shibo Shao , Ke Wang , Yiming Zhang , Jason B. Love , Zongyang Yue , Wei Li , Liangliang Huang , Yuyin Wang , Xiaokun Yao , Tianxiao Chang , Xianfeng Fan

Photocatalytic conversion of lignin into aromatic monomers by cleaving interunit C–O bonds is a promising approach to reduce reliance on fossil fuel resource. However, industrial implementation is hindered by insufficient reaction efficiency and selectivity for target monomers. This study addresses these challenges by applying adsorbent-mediated catalysis and developing a quaternary CdxZn1–xIn2S4 photocatalyst. This catalyst utilizes radical species from photocatalytic water dissociation to promote the cleavage of aryl ether C–O bonds in lignin model compounds, achieving nearly complete conversion with over 90% selectivity for target aromatic monomers. This is a significant improvement over the 50% or less conversion and selectivity performed by water-free photocatalytic system. The study shows that H∗ and ∗OH from water dissociation can modify the catalytic microenvironment and reaction kinetics, increasing the energy barrier for side reactions and enhancing hydrogen transfer efficiency. Therefore, the target C–O cleavages can be remarkably promoted while the oxy-dehydrogenation side reactions can be impeded.



中文翻译:


利用水离解自由基物质吸附剂将木质素光催化转化为芳香族单体



通过裂解单元间 C-O 键将木质素光催化转化为芳香族单体是减少对化石燃料资源依赖的一种有前景的方法。然而,反应效率和目标单体选择性不足阻碍了工业实施。本研究通过应用吸附剂介导的催化并开发四元 Cd x Zn 1– x In 2 S 4光催化剂来解决这些挑战。该催化剂利用光催化水解离产生的自由基物种来促进木质素模型化合物中芳基醚C-O键的裂解,实现几乎完全转化,对目标芳香族单体的选择性超过90%。与无水光催化系统所实现的 50% 或更低的转化率和选择性相比,这是一个显着的改进。研究表明,水解离产生的H*和*OH可以改变催化微环境和反应动力学,增加副反应的能垒并提高氢转移效率。因此,可以显着促进目标C-O裂解,同时可以阻止氧化脱氢副反应。

更新日期:2024-07-23
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