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Efficient photocatalytic one-pot hydrogenation and N-alkylation of nitrobenzenes/benzonitriles with alcohols over Pd/MOFs: Effect of the crystal morphology & "quasi-MOF" structure
被引:42
|作者:
Cheng, Hongmei
[1
]
Long, Xingyu
[1
]
Bian, Fengxia
[1
]
Yang, Chaofen
[2
]
Liu, Xingyan
[1
]
Jiang, Heyan
[1
]
机构:
[1] Chongqing Technol & Business Univ, Coll Environm & Resources, Natl Base Int Sci & Technol Cooperat Intelligent, Chongqing Key Lab Catalysis & New Environm Mat, Chongqing 400067, Peoples R China
[2] Kunming Univ Sci & Technol, Res Ctr Anal & Measurement, Kunming 650093, Yunnan, Peoples R China
基金:
中国国家自然科学基金;
关键词:
Photocatalysis;
Pd/quasi-MOF;
N-Alkylation;
Nitrobenzenes;
Benzonitriles;
METAL-ORGANIC FRAMEWORKS;
FE-BASED MOFS;
BENZYL ALCOHOL;
2-METHYLIMIDAZOLE-ASSISTED SYNTHESIS;
SELECTIVE OXIDATION;
CATALYTIC-ACTIVITY;
PD NANOPARTICLES;
MIL-101;
AMINES;
REDUCTION;
D O I:
10.1016/j.jcat.2020.05.033
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:
One-pot multi-step reactions over visible-light induced catalysis feature the sustainable green process. Here, ligand structure change and 2-MI coordinated modulation were adapted to adjust the crystal size, morphology and crystalline structure of Fe-MOFs; double solvent impregnation was employed for the Pd loading; "quasi-MOF" materials with retained morphology were formed with calcination under N-2. Above modified materials were employed as multifunctional photocatalysts for highly efficient one-pot hydrogenation and N-alkylation of nitrobenzenes or benzonitriles with alcohols after in situ Pd photoreduction. Photocatalytic performance was evidently affected by the Fe-MOFs crystal size, morphology, crystalline structure alteration and "quasi-MOF" construction. One-pot hydrogenation and N-alkylation of benzonitriles with alcohols was achieved with excellent catalytic performance firstly in heteroegeneous catalysis. Reaction mechanism was proposed with the assistance of in situ DRIFTS. (C) 2020 Elsevier Inc. All rights reserved.
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页码:121 / 131
页数:11
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