Highly effective synthesis of dimethyl carbonate over CuNi alloy nanoparticles @Porous organic polymers composite

Chen, Yongdong; Yang, You; Tian, Shanli; Ye, Zhongbin; Tang, Qiang; Lin, Yuzhen; Li, Gao

doi:10.1016/j.apcata.2019.117275

Cited by 36 publications

(25 citation statements)

References 51 publications

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“…Aer the 24 hour period, a small decrease in the amount of DMC yield was observed reaching 26.2% (entry 11, Table 1). According to literature, 28 water withdrawal from the reaction medium has great interference in the DMC synthesis optimization time since smaller amount of water allows greater catalytic activity and catalyst durability. From these results one can infer that the molecular sieve porosity improved catalytic activity and increased DMC production by withdrawing the water produced during the reaction.…”

Section: Resultsmentioning

confidence: 99%

Dehydrating agent effect on the synthesis of dimethyl carbonate (DMC) directly from methanol and carbon dioxide

et al. 2020

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Section: Resultsmentioning

confidence: 99%

Dehydrating agent effect on the synthesis of dimethyl carbonate (DMC) directly from methanol and carbon dioxide

et al. 2020

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“…It is continuously examined more than 115 hours under 140°C and 2.4 MPa and the test result is noted in Figure 10b. It shows the CH 3 OH conversion and DMC selectivity are almost constant at ~22% and ~80%, respectively, and no deactivation is observed during the catalytic test of the initial 100 hours, which indicates that the durability of the Ce 0.95 La 0.05 O δ monolithic catalyst is as high as 100 hours, which is much higher than that of Cu 1 Ni 1 @POP-PPh 3 monolithic catalyst (about 16 hours) [20] and Ti 0.1 Ce 0.9 O 2 monolithic catalyst (less than 50 hours) [14]. However, after the 100 hours' catalytic reaction, the conversion of CH 3 OH and the selectivity of DMC decrease slightly to 20% and 76%, respectively.…”

Section: Catalytic Performancementioning

confidence: 90%

“…This is mainly due to the following facts that the by-product water can be quickly detached from the surface of the monolithic catalyst during the reaction process, thus avoiding the catalyst activity reduction or even deactivation due to water poisoning. In all, the catalysts uniformly coated onto the honeycomb ceramics indeed can largely improve the catalytic performance (including the CH 3 OH conversion and selectivity toward target product dimethyl carbonate) in the direct dimethyl carbonate synthesis reactions investigated in the direct DMC synthesis at 140 °C, Figure 10a [8,16,20,47,48]. This is mainly attributed to the monolithic catalysts can reduce the interaction between catalyst and gas (including reactants and products) and remove the generated water in time, thus improving the catalytic activity.…”

Section: Catalytic Performancementioning

confidence: 93%

“…It has been reported that many nano-catalysts were effective for increasing the yield of this reaction, such as supported Cu-Ni bimetallic catalysts [18][19][20], organometallic compounds [21], zirconium oxide [22], cerium oxide [23,24], CeO 2 -ZrO 2 [5,25,26], and so on. According to the catalysts reported in the literature, transition metal-doped ceria catalysts showed excellent catalytic activity [5].…”

Section: Introductionmentioning

confidence: 99%

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Lanthanum-Doped Ceria Nanocomposite: A Highly Stable Monolithic Catalyst for Direct Synthesis of Dimethyl Carbonate

Chen¹,

Ye²,

Li³

et al. 2020

JEECE

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That dimethyl carbonate is directly synthesized from methanol and carbon dioxide is an effective and environmental approach to solve the greenhouse effect. For the sake of solving the problems of low DMC productivity and poor catalysts stability in presence of the formed water. Here we design and prepare a serial of spherical La-doped ceria nanoparticles (Ce 1-x La x O δ nanocomposites, x=0.00, 0.05, 0.10, 0.15, and 0.20) via a co-precipitation method. These Ce 1-x La x O δ composites are ground into slurry by ball milled and then coated on cordierite honeycomb ceramics to obtain Ce 1-x La x O δ monolithic catalysts. These Ce 1-x La x O δ composites are characterized extensively by TEM, XRD, Raman spectroscopy, N 2 adsorption-desorption isotherms, H 2 -TPR and XPS. The characterization results show that the Ce 1-x La x O δ composites nanoparticles possesses richer surface oxygen vacancies, higher BET surface area and smaller particle size than that of pure CeO 2 nanoparticle. Besides, catalytic activity test shows these Ce 1-x La x O δ monolithic catalysts exhibit better catalytic performance than that of pure CeO 2 nanoparticles. Among them, Ce 0.95 La 0.05 O δ monolithic catalyst exhibits the highest CH 3 OH conversion and DMC yield, which is in good line with the oxygen vacancy content measured by XPS. Finally, the Ce 0.95 La 0.05 O δ monolithic catalyst also shows an excellent durability of more than 100 hours, which is mainly due to the doping effect of lanthanum into the ceria oxides tailoring the structure and surface properties of the catalyst.

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“…To the best of our knowledge Bi-doped ceria has so far not been evaluated as potential catalyst for the direct DMC synthesis [16]. The use of honeycomb-type catalysts could offer several advantages compared to fixed-beds of related particulate catalysts [24][25][26]. Monolithic catalysts exhibit good interphase mass and heat transfer, low pressure drop at relatively large surface area, and could facilitate more efficient removal of the formed by-product (water), which unfavorably affects the thermodynamic equilibrium and limits the catalytic efficiency of the DMC synthesis [27].…”

Section: Introductionmentioning

confidence: 99%

Continuous dimethyl carbonate synthesis from CO2 and methanol over BixCe1−xOδ monoliths: Effect of bismuth doping on population of oxygen vacancies, activity, and reaction pathway

Chen

et al. 2021

Nano Res.

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We evaluated bismuth doped cerium oxide catalysts for the continuous synthesis of dimethyl carbonate (DMC) from methanol and carbon dioxide in the absence of a dehydrating agent. BixCe1−xOδ nanocomposites of various compositions (x = 0.06–0.24) were coated on a ceramic honeycomb and their structural and catalytic properties were examined. The incorporation of Bi species into the CeO2 lattice facilitated controlling of the surface population of oxygen vacancies, which is shown to play a crucial role in the mechanism of this reaction and is an important parameter for the design of ceria-based catalysts. The DMC production rate of the BixCe1−xOδ catalysts was found to be strongly enhanced with increasing Ov concentration. The concentration of oxygen vacancies exhibited a maximum for Bi0.12Ce0.88Oδ, which afforded the highest DMC production rate. Long-term tests showed stable activity and selectivity of this catalyst over 45 h on-stream at 140 °C and a gas-hourly space velocity of 2,880 mL·gcat−1·h−1. In-situ modulation excitation diffuse reflection Fourier transform infrared spectroscopy and first-principle calculations indicate that the DMC synthesis occurs through reaction of a bidentate carbonate intermediate with the activated methoxy (−OCH3) species. The activation of CO2 to form the bidentate carbonate intermediate on the oxygen vacancy sites is identified as highest energy barrier in the reaction pathway and thus is likely the rate-determining step.

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Highly effective synthesis of dimethyl carbonate over CuNi alloy nanoparticles @Porous organic polymers composite

Cited by 36 publications

References 51 publications

Dehydrating agent effect on the synthesis of dimethyl carbonate (DMC) directly from methanol and carbon dioxide

Dehydrating agent effect on the synthesis of dimethyl carbonate (DMC) directly from methanol and carbon dioxide

Lanthanum-Doped Ceria Nanocomposite: A Highly Stable Monolithic Catalyst for Direct Synthesis of Dimethyl Carbonate

Continuous dimethyl carbonate synthesis from CO2 and methanol over BixCe1−xOδ monoliths: Effect of bismuth doping on population of oxygen vacancies, activity, and reaction pathway

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