Study of Thermodynamics and Experiment on Direct Synthesis of Dimethyl Carbonate from Carbon Dioxide and Methanol over Yttrium Oxide

Abstract

The thermodynamics on the direct synthesis of dimethyl carbonate (DMC) from CO2 and CH3OH was calculated and analyzed. Using Y­(NO3)3·6H2O as the precursor, a series of Y2O3 were prepared through the one-pot calcination method, which were employed to catalyze DMC synthesis. The decomposition temperature of Y­(NO3)3·6H2O was measured by thermogravimetric analysis, and Y2O3 was obtained after the precursor calcination at desired temperatures, denoted as Y2O3-T (°C). The catalysts were characterized by X-ray diffraction, Brunauer–Emmett–Teller method, transmission electron microscopy, NH3/CO2 temperature-programmed desorption, and X-ray photoelectron spectroscopy to detect the crystal phase, surface property, particle size, acidity–basicity amounts, and oxidation state, respectively. The characterization results indicated that Y2O3-750 can favor the formation of moderate acidic and basic sites and facilitate the activation of CO2 and CH3OH. The catalytic performance evaluation was experimentally investigated, and Y2O3-750 owned the highest DMC yield of 1.02 mmol/g·cat under 90 °C, 8 MPa, and 6 h, which also exhibited reliable recycle ability.

Reaction of CO2 With Alcohols to Linear-, Cyclic-, and Poly-Carbonates Using CeO2-Based Catalysts

“…Other ZrO 2 -based catalysts have been studied ( Table 2, Entries 5-7) and the activity seems to be comparable to that in previous reports (Zhang et al, 2014;Li et al, 2017;Akune et al, 2018). It has been recently reported that Y 2 O 3 was an effective catalyst for the DMC synthesis from CO 2 and methanol ( Table 2, Entry 8), and it is characteristic that Y 2 O 3 has some activity at lower reaction temperature (363 K) than usual (for example, 383-423 K) (Sun et al, 2020). Unfortunately, the formation rate of DMC is not determined on Y 2 O 3 precisely, and the formation rate can be clearly higher than the estimated value.…”

Surface effect of nano-sized cerium-zirconium oxides for the catalytic conversion of methanol and CO2 into dimethyl carbonate

“…Current state of the art of DMC synthesis over ceria-based catalysts is detailed elsewhere [28]. Among rare earth oxide elements, Y 2 O 3 was also reported [29] to catalyze DMC synthesis at 353 K, one of the lower temperature reported for this reaction.…”

From ‘Gift’ to gift: producing organic solvents from CO2

“…Wang and co-workers prepared a series of Y 2 O 3 -T catalysts through a one-pot calcination method from Y(NO 3 ) 3 •6H 2 O and applied them to study the thermodynamics of the direct synthesis of DMC from CO 2 . 171 The efficiency of DMC formation was closely related to the moderate acidity-basicity amounts of the catalysts. Y 2 O 3 -750 showed the best catalytic performance to give the highest yield of DMC at 90 °C under 8 MPa of CO 2 .…”