Reduction of carbon dioxide to dimethylformamide using ruthenium doped Mg/Al hydrotalcites under supercritical conditions

被引:1
作者
Chaudhary, Sagar D. [1 ,2 ]
Rahatade, Shardul S. [1 ]
Joshi, Sunil S. [1 ,2 ]
Mali, Nilesh A. [1 ,2 ]
机构
[1] CSIR, Natl Chem Lab, Chem Engn & Proc Dev, Pune 411008, India
[2] Acad Sci & Innovat Res AcSIR, Ghaziabad 201002, India
关键词
Hydrotalcite; Supercritical carbon dioxide; Hydrogenation; Dimethylformamide; Langmuir-Hinshelwood-Hougen-Watson model; RHODIUM-CATALYZED HYDROGENATION; HYBRID GEL CATALYSTS; FORMIC-ACID; CHEMICAL-REACTIONS; HOMOGENEOUS HYDROGENATION; SELECTIVE HYDROGENATION; ANIONIC CLAYS; CO2; COMPLEXES; N; N-DIMETHYLFORMAMIDE;
D O I
10.1016/j.jcou.2022.102055
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The utilization of carbon dioxide is one of the developing areas due to its significant contribution to global warming. Reducing carbon dioxide (CO2) to formic acid and its derivatives has gained importance because of its thermodynamic limitations and high industrial demand. In this article, we report the synthesis of dime-thylformamide (DMF) using ruthenium doped Mg/Al calcined hydrotalcite by CO2 hydrogenation in the presence of dimethylamine (DMA). At optimized conditions, complete conversion of dimethylamine was achieved with more than 92% product yield at 170 degrees C and 13 MPa pressure with a reaction time of 6 h. Key catalyst properties were determined using X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), CO2-temper-ature programmed desorption (TPD), H-2 temperature-programmed reduction (TPR) and Fourier transform infrared (FTIR). The determination of surface morphology was carried out using field emission scanning electron microscope (FE-SEM) and high-resolution transmission electron microscopy (HR-TEM). At the same time, the chemical composition was verified by energy-dispersive X-ray (EDS). In addition, kinetic modeling is performed using the two site Langmuir-Hinshelwood-Hougen-Watson model. The regressed kinetic parameters gave an appropriate fit with experimental concentration values and activation energy is calculated as 413 kJ/mol K-1.
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页数:10
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共 54 条
[1]   Selective Synthesis of Secondary and Tertiary Amines by Reductive N-Alkylation of Nitriles and N-Alkylation of Amines and Ammonium Formate Catalyzed by Ruthenium Complex [J].
Alshakova, Iryna D. ;
Nikonov, Georgii, I .
CHEMCATCHEM, 2019, 11 (21) :5370-5378
[2]   Ni or Ru supported on MgO/-Al2O3 pellets for the catalytic conversion of ethanol into butanol [J].
Apuzzo, J. ;
Cimino, S. ;
Lisi, L. .
RSC ADVANCES, 2018, 8 (45) :25846-25855
[3]   New hydrotalcite-type anionic clays containing noble metals [J].
Basile, F ;
Basini, L ;
Fornasari, G ;
Gazzano, M ;
Trifiro, F ;
Vaccari, A .
CHEMICAL COMMUNICATIONS, 1996, (21) :2435-2436
[4]   Synthesis and thermal evolution of hydrotalcite-type compounds containing noble metals [J].
Basile, F ;
Fornasari, G ;
Gazzano, M ;
Vaccari, A .
APPLIED CLAY SCIENCE, 2000, 16 (3-4) :185-200
[5]   Catalytic Hydrogenation of Carbon Dioxide to Formic Acid [J].
Behr, Arno ;
Nowakowski, Kristina .
CO2 CHEMISTRY, 2014, 66 :223-258
[6]   Catalytic hydrogenation in supercritical CO2: Kinetic measurements in a gradientless internal-recycle reactor [J].
Bertucco, A ;
Canu, P ;
Devetta, L ;
Zwahlen, AG .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1997, 36 (07) :2626-2633
[7]   Review of the synthesis of layered double hydroxides:: A thermodynamic approach [J].
Bravo-Suárez, JJ ;
Páez-Mozo, EA ;
Oyama, ST .
QUIMICA NOVA, 2004, 27 (04) :601-614
[8]   HYDROTALCITE-TYPE ANIONIC CLAYS: PREPARATION, PROPERTIES AND APPLICATIONS [J].
Cavani, F. ;
Trifiro, F. ;
Vaccari, A. .
CATALYSIS TODAY, 1991, 11 (02) :173-301
[9]   Methylamines synthesis: A review [J].
Corbin, DR ;
Schwarz, S ;
Sonnichsen, GC .
CATALYSIS TODAY, 1997, 37 (02) :71-102
[10]   DETERMINATION OF BASE PROPERTIES OF HYDROTALCITES - CONDENSATION OF BENZALDEHYDE WITH ETHYL ACETOACETATE [J].
CORMA, A ;
FORNES, V ;
MARTINARANDA, RM ;
REY, F .
JOURNAL OF CATALYSIS, 1992, 134 (01) :58-65