Highly efficient NiCo alloy catalyst fabricated by MOFs-templated strategy for N-formylation reaction of amines with CO2 and phenylsilane

被引:1
作者
Li, Qixuan [1 ]
Li, Yufei [1 ]
Fu, Rui [2 ]
Gong, Dawei [1 ]
Song, Wenjing [2 ]
Li, Weizuo [2 ]
Wang, Xin [3 ]
机构
[1] Jilin Normal Univ, Coll Chem, Minist Educ, Key Lab Preparat & Applicat Environm Friendly Mat, Changchun 130103, Peoples R China
[2] Changzhou Univ, Sch Petrochem Engn, Changzhou 213164, Jiangsu, Peoples R China
[3] Jiangnan Univ, Med Ctr, Wuxi 214002, Jiangsu, Peoples R China
来源
MOLECULAR CATALYSIS | 2025年 / 575卷
基金
国家教育部博士点专项基金资助;
关键词
MOFs templated method; NiCo alloy catalysts; N-formylation reaction; METAL-ORGANIC FRAMEWORKS; CARBON-DIOXIDE; METHYLATION;
D O I
10.1016/j.mcat.2025.114896
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
N-formylation of amines with carbon dioxide (CO2) and phenylsilane represents a sustainable and efficient pathway for synthesizing nitrogen-containing compounds, leveraging the growing interest in using CO2 as a feedstock in organic synthesis. Based on a bimetallic MOFs templating approach, this study synthesized an efficient NiCo alloy catalyst (termed as NiCo/CN-hmta) for the N-formylation reaction of phenylsilane, CO2, and N-methylbenzene amine. The catalytic performance results indicate that the NiCo/CN-hmta catalyst exhibits high catalytic activity in the N-formylation reaction process. Various characterizations and comparative experiments to explore the reasons for the enhancement in performance of NiCo/CN-hmta for N-formylation reaction. Additionally, there remain many speculative reaction pathways during the N-formylation reaction, and there is significant controversy regarding the order of interactions among phenylsilane, CO2, and N-methylbenzene amine. Therefore, this study aims to determine the reaction pathway of the MOFs-derived NiCo alloy catalyst in the N-formylation reaction through deuterated experiments, In-situ diffuse reflection infrared Fourier transform spectroscopy (in-situ DRIFTS) and 13C NMR tests to capture intermediates during the reaction process. We hope that our research can provide some insights for future applications of alloy catalysts in N-formylation reactions.
引用
收藏
页数:9
相关论文
共 66 条
[21]   Mechanistic Insights into a Co(II)-Coordinated "Free" Metal Site of 2D Zinc-Based MOFs for β-Alkylation of Secondary Alcohols with Primary Alcohols [J].
Li, Weizuo ;
Fu, Rui ;
Shi, Jing ;
Xiao, Zhenhao ;
Xu, Yue ;
He, Dafang ;
He, Guangyu ;
Chen, Haiqun ;
Xie, Mingchen .
INORGANIC CHEMISTRY, 2023, 62 (45) :18689-18696
[22]   A Banana-like Ni-MgO Solid Solution Catalyst Derived from Bimetallic Ni-Mg@MOFs for Hydrogenation of Nitroarenes [J].
Li, Weizuo ;
Fu, Rui ;
Luo, Xue ;
Wang, Xin .
CURRENT ORGANIC CHEMISTRY, 2023, 27 (06) :465-470
[23]   Boosting performance for hydrogenation-alkylation tandem reaction catalyzed by banana-like MgO-based solid solution confined Ni-Co alloy catalyst: Fabricated by a MTV-MOFs templated strategy [J].
Li, Weizuo ;
Wang, Jing ;
He, Dafang ;
He, Guangyu ;
Chen, Haiqun .
MOLECULAR CATALYSIS, 2022, 529
[24]  
Li X., 2025, Appl. Organomet. Chem., V39, P7974
[25]   Design of Lewis base functionalized ionic liquids for the N-formylation of amines with CO2 and hydrosilane: The cation effects [J].
Li, Xiao-Ya ;
Fu, Hong-Chen ;
Liu, Xiao-Fang ;
Yang, Shu-Han ;
Chen, Kai-Hong ;
He, Liang-Nian .
CATALYSIS TODAY, 2020, 356 :563-569
[26]   Copper catalysis: ligand-controlled selective N-methylation or N-formylation of amines with CO2 and phenylsilane [J].
Li, Xue-Dong ;
Xia, Shu-Mei ;
Chen, Kai-Hong ;
Liu, Xiao-Fang ;
Li, Hong-Ru ;
He, Liang-Nian .
GREEN CHEMISTRY, 2018, 20 (21) :4853-4858
[27]   A highly efficient LaOCl supported Fe-Fe3C-based catalyst for hydrogenation of nitroarenes fabricated by coordination-assisted pyrolysis [J].
Li, Xuewei ;
She, Wei ;
Wang, Jing ;
Li, Weizuo ;
Li, Guangming .
CATALYSIS SCIENCE & TECHNOLOGY, 2021, 11 (13) :4627-4635
[28]   Highly efficient N-doped carbon supported FeSx-Fe2O3 catalyst for hydrogenation of nitroarenes via pyrolysis of sulfurized N,Fe-containing MOFs [J].
Li, Xuewei ;
She, Wei ;
Wang, Jing ;
Li, Weizuo ;
Li, Guangming .
APPLIED ORGANOMETALLIC CHEMISTRY, 2021, 35 (08)
[29]   Ruthenium Single-Atom Anchored in Polyoxometalate-Ionic Liquids for N-Formylation of Amines with CO2 and H2 [J].
Ma, Yuan ;
Chen, Chen ;
Jiang, Yongjun ;
Wei, Xinjia ;
Liu, Ying ;
Liao, Huiying ;
Wang, Haifeng ;
Dai, Sheng ;
An, Pengfei ;
Hou, Zhenshan .
ACS CATALYSIS, 2023, 13 (15) :10295-10308
[30]   Critical Role of CUS in the Au/MOF-808(Zr) Catalyst for Reaction of CO2 with Amine/H2 via N-Methylation and N-Formylation [J].
Mu, Jincheng ;
Liu, Jianfang ;
Ran, Zhenzhen ;
Arif, Muhammad ;
Gao, Min ;
Wang, Chen ;
Ji, Shengfu .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2020, 59 (14) :6543-6555