Modulation of ketyl radical reactivity to mediate the selective synthesis of coupling and carbonyl compounds

被引：2
|
作者：
Chen, Zhaohui [1 ]
Deng, Jun [1 ]
Zheng, Yanmei [1 ]
Zhang, Wenjun [1 ]
Dong, Lin [1 ]
Chen, Zupeng [1 ]
机构：
[1] Nanjing Forestry Univ, Coll Chem Engn, Jiangsu Coinnovat Ctr Efficient Proc & Utilizat Fo, Int Innovat Ctr Forest Chem & Mat, Nanjing 210037, Jiangsu, Peoples R China
来源：
CHINESE JOURNAL OF CATALYSIS | 2024年 / 61卷
基金：
中国博士后科学基金;
关键词：
Biomass valorization; Photocatalysis; Ketyl radical reactivity; Selectivity control; Adsorption energy; TOTAL-ENERGY CALCULATIONS; PHOTOCATALYTIC CONVERSION; LIGNOCELLULOSIC BIOMASS; BENZYL ALCOHOL; COCATALYST; OXIDATION; H-2;
D O I：
10.1016/S1872-2067(24)60045-8
中图分类号：
O69 [应用化学];
学科分类号：
081704 ;
摘要：
The importance of selective synthesis of high-value-added chemicals from renewable resources is paramount but remains a crucial challenge in organic synthesis and chemical reformation. Herein, we report the selective photosynthesis of C-C coupling products and carbonyl compounds from biomass-derived alcohols. The key to ensuring high end-to-end selectivity is the modulation of the reactivity of ketyl radical (*RCHOH) intermediates by employing different metal co-catalysts (Au, Pt, Pd, Ru) supported on Cd0.6Zn0.4S solid solution (CZS) photocatalysts. In particular, the C-C coupling product, hydrobenzion, and fully oxidized benzaldehyde were obtained from benzyl alcohol with high selectivity (> 98%) over Au-CZS and Ru-CZS, respectively. Combined experimental and theoretical analyses demonstrated that the affinity of *RCHOH for the surface of metals governs their subsequent transformations, in which weak and strong radical adsorption on Au and Ru results in C-C coupling products and carbonyl compounds, respectively. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved..
引用
收藏
页码：135 / 143
页数：9
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