铌基催化剂精准活化木质素C(aromatic)-C键的催化本质研究
批准号:
22002043
项目类别:
青年科学基金项目
资助金额:
24.0 万元
负责人:
董琳
依托单位:
学科分类:
催化化学
结题年份:
2023
批准年份:
2020
项目状态:
已结题
项目参与者:
董琳
中文摘要
木质素催化氢解制备芳香类化学品具有广泛的工业应用前景,而氢解过程中C-C键的精准活化是提高木质素碳利用率的关键。我们在前期研究中发现,Ru/Nb基催化剂具有选择氢解C(aromatic)-C键,同时抑制其它类型C-C键断裂的特性。本项目拟从NbOx对C(aromatic)-C键的精准活化,及NbOx与Ru的相互作用对C(aromatic)-C键的选择性氢解出发,考察不同氧化物负载的Ru催化剂在苯基环己烷氢解反应中的催化性能,探究铌基材料在C(aromatic)-C键氢解中独特作用;研究模型分子在铌基材料表面的吸附、活化和氢解过程,充分认识铌基材料在C(aromatic)-C键活化中的作用本质;对比不同金属/氧化物的物化性质和催化性能,深入理解加氢中心Ru与C-C键活化中心NbOx在苯基环己烷氢解反应中的协同机制,为靶向合成具有C(aromatic)-C键活化性能的高效催化剂提供新思路。
英文摘要
The preparation of aromatic chemicals by catalytic hydrogenolysis of lignin has broad industrial application prospect, and the precise activation of C-C linkages in the hydrogenolysis of lignin is the key to enhance the utilization ratio of carbon in lignin. In our previous studies, we found that the Ru/NbOx catalyst has excellent activity for selective hydrogenolysis of C(aromatic)-C bonds, meanwhile it avoids the cleavage of other C-C bonds. This project intends to start with the precise activation of C(aromatic)-C bonds by NbOx and the selective hydrogenolysis by a synergistic effect between NbOx and Ru, by compared with catalyst performance of various oxides loaded Ru-based catalysts in the hydrogenolysis of phenylcyclohexane, in order to explore the unique role of NbOx in hidrogenolysis of C(aromatic)-C bonds. The adsorption, binding and reaction of phenylcyclohexane on niobium-based catalyst will be studied, in order to explore the nature of the role of niobium-based materials in the activation of C(aromatic)-C bonds. Reveal the synergetic mechanism of hydrogenation centers Ru and C-C activation centers NbOx in the hydrogenolysis of phenylcyclohexane, through studying physicochemical property and catalyst performance of various oxides loaded Ru-based catalysts. Meanwhile, the relationship between catalyst composition structure and performance will be established. It would be believed to provide a novel idea for the controlled synthesis of excellent catalyst with precise C(aromatic)-C activation and hydrogenolysis.
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DOI:
10.1016/j.jcat.2023.115241
发表时间:
2023-12
期刊:
Journal of Catalysis
影响因子:
7.3
作者:
[Yiwen Zou;Lin Dong;Siyang Yan;Jiaxu Liu;Lili Mu;Licheng Li;Yue Hu;Haifeng Qi;Shanjun Mao;Zupeng Chen]
通讯作者:
Yiwen Zou;Lin Dong;Siyang Yan;Jiaxu Liu;Lili Mu;Licheng Li;Yue Hu;Haifeng Qi;Shanjun Mao;Zupeng Chen
DOI:
10.1038/s41467-022-31362-9
发表时间:
2022-06-27
期刊:
Nature communications
影响因子:
16.6
作者:
[]
通讯作者:
DOI:
10.1016/j.apcatb.2023.122893
发表时间:
2023-05
期刊:
Applied Catalysis B: Environmental
影响因子:
--
作者:
[Lin Dong;Jordi Morales‐Vidal;Lili Mu;Licheng Li;N. López;J. Pérez–Ramírez;Zupeng Chen]
通讯作者:
Lin Dong;Jordi Morales‐Vidal;Lili Mu;Licheng Li;N. López;J. Pérez–Ramírez;Zupeng Chen
DOI:
--
发表时间:
2023
期刊:
Green Chemistry
影响因子:
作者:
[Yuguo Dong, Lin Dong, Xiaoli Gu, Yanqin Wang, Yuhe Liao, Rafael Luque, Zupeng Chen]
通讯作者:
Zupeng Chen
Mechanisms of Caromatic-C bonds cleavage in lignin over NbOx-supported Ru catalyst
NbOx 负载 Ru 催化剂上木质素中芳香族 C 键断裂的机制
DOI:
10.1016/j.jcat.2021.01.001
发表时间:
2021-01-25
期刊:
JOURNAL OF CATALYSIS
影响因子:
7.3
作者:
[Dong, Lin, Xia, Jie, Wang, Yanqin]
通讯作者:
Wang, Yanqin
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国内基金
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