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光催化有机溶木质素解聚制备有价值化学品。

Photocatalytic depolymerization of organosolv lignin into valuable chemicals.

机构信息

Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China; College of Material and Chemical Engineering, Chuzhou University, Chuzhou, Anhui 239000, China.

Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China.

出版信息

Int J Biol Macromol. 2021 Jun 1;180:403-410. doi: 10.1016/j.ijbiomac.2021.03.067. Epub 2021 Mar 17.

DOI:10.1016/j.ijbiomac.2021.03.067
PMID:33741371
Abstract

Catalytic conversion of lignin to certain aromatic compounds has been extensively studied but still has great challenges. Photocatalytic depolymerizing lignin is a very promising method to obtain valuable chemicals. Herein, ZnInS (ZIS)-based photocatalyst was successfully synthesized by simply combining ZIS and graphene oxide (GO). Photocatalyst ZIS-100 can efficiently depolymerize organosolv lignin into phenols and ketones. The relative content of valuable compounds in the depolymerized product was increased by 2.5 times as compared that without photocatalyst. The photocatalyst can effectively break C-O bonds in 2-phenoxy-1-phenylethanol (PP-ol, a model compound) and the conversion of PP-ol is 93.27%. Mechanism studies show that the thiol groups on the surface of ZIS-100 play an important role in the formation of C radical intermediates. Photocatalytic cleavage of C-O bond mainly follows a one-step reaction mechanism through a self‑hydrogen transfer process. This study provides a new strategy for selectively breaking C-O bond in lignin to form valuable chemicals.

摘要

木质素转化为某些芳香族化合物的催化转化已得到广泛研究,但仍面临巨大挑战。光催化解聚木质素是获得有价值化学品的一种很有前途的方法。在此,通过简单地将 ZnInS(ZIS)和氧化石墨烯(GO)结合,成功合成了基于 ZIS 的光催化剂。光催化剂 ZIS-100 可以有效地将有机溶剂木质素解聚成酚类和酮类物质。与没有光催化剂相比,解聚产物中有价值化合物的相对含量增加了 2.5 倍。该光催化剂可以有效地打断 2-苯氧基-1-苯乙醇(PP-ol,一种模型化合物)中的 C-O 键,其转化率为 93.27%。机理研究表明,ZIS-100 表面的巯基在 C 自由基中间体的形成中起重要作用。C-O 键的光催化断裂主要通过自氢转移过程遵循一步反应机理。本研究为选择性打断木质素中的 C-O 键以形成有价值的化学品提供了一种新策略。

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