Pd/N-doped carbon dots@dendritic mesoporous silica nanospheres: A highly efficient catalyst for the hydrogenation of 4-nitrophenol

被引:4
作者
Liu, Weiruo [1 ]
Zhu, Yanbin [2 ,3 ]
Wang, Jiwei [2 ,3 ]
Feng, Haisong [4 ]
Zhai, Yunpu [1 ]
Li, Wei [2 ,3 ]
Zhao, Dongyuan [2 ,3 ]
机构
[1] Zhengzhou Univ, Coll Chem, 100 Kexue Ave, Zhengzhou 450001, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Adv Mat Lab, Dept Chem, Shanghai 200433, Peoples R China
[3] Fudan Univ, State Key Lab Mol Engn Polymers, Shanghai 200433, Peoples R China
[4] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
palladium nanoparticles; nitrogen-doped carbon dots; dendritic mesoporous silica; catalytic hydrogenation; 4-nitrophenol reduction; TOTAL-ENERGY CALCULATIONS; PALLADIUM NANOPARTICLES; FORMIC-ACID; OXIDATION; DEHYDROGENATION; REDUCTION;
D O I
10.1007/s12274-024-6809-9
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Highly dispersed Pd/N-doped carbon dots (Pd/NCDs) were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres (NMS). The synthesized Pd/NCDs@NMS catalyst exhibits outstanding performance in the catalytic reduction of 4-nitrophenol (4-NP), achieving a turnover frequency of 1461.8 mol<middle dot>molPd-1<middle dot>h-1, with the conversion rate remaining above 80% after 11 cycles. Experiments and density functional theory calculations reveal that the NCDs significantly affect the electronic structure of Pd nanoparticles, leading to changes in the energy barriers for the adsorption of 4-NP at the Pd sites and the conversion of 4-NP reaction intermediates, which is a key factor contributing to the catalytic performance. This study offers a new strategy for synthesizing carbon-dot-modified metal-based catalysts.
引用
收藏
页码:7967 / 7974
页数:8
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