Tailoring the Porous Structure of Carbon for Enhanced Oxidative Cleavage and Esterification of C(CO)-C Bonds.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2024-12-29 DOI:10.1002/cssc.202402553
Chao Xie, Qidong Hou, Hengli Qian, Yao Tang, Ruite Lai, Xinyu Bai, Guanjie Yu, Shuai Lv, Tianliang Xia, Zejun Liu, Xin Huang, Xiaojun Shen, Meiting Ju
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Abstract

The cleavage and functionalization of carbon-carbon bonds are crucial for the reconstruction and upgrading of organic matrices, particularly in the valorization of biomass, plastics, and fossil resources. However, the inherent kinetic inertness and thermodynamic stability of C-C σ bonds make this process challenging. Herein, we fabricated a glucose-derived defect-rich hierarchical porous carbon as a heterogeneous catalyst for the oxidative cleavage and esterification of C(CO)-C bonds. Systematic investigations revealed that the hierarchical porous structure enhances the adsorption of O2 and ketones, thereby boosting the catalytic efficiency of defects. This catalyst exhibits performance comparable to that of the reported nitrogen-doped or metal nanoparticle-supported carbon materials, as well as transition metal-based homogeneous catalytic systems. This work deepens our understanding of the reaction process underlying this transformation and provides insights for designing efficient carbon-based materials for oxidative transformations.

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调整碳的多孔结构以增强C(CO)-C键的氧化裂解和酯化反应。
碳-碳键的裂解和功能化对于有机基质的重建和升级至关重要,特别是在生物质、塑料和化石资源的增值中。然而,C-C σ键固有的动力学惰性和热力学稳定性使得这一过程具有挑战性。在此,我们制备了一种葡萄糖衍生的富含缺陷的分层多孔碳作为C(CO)-C键氧化裂解和酯化的非均相催化剂。系统研究表明,分层多孔结构增强了对O2和酮类的吸附,从而提高了缺陷的催化效率。该催化剂表现出与已有报道的氮掺杂或金属纳米颗粒支撑的碳材料以及过渡金属基均相催化系统相当的性能。这项工作加深了我们对这种转化背后的反应过程的理解,并为设计用于氧化转化的高效碳基材料提供了见解。
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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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