Direct dimethyl carbonate synthesis from CO2 and methanol over a flower-like CeO2 catalyst with 2-cyanopyridine as a dehydrating agent in continuous packed-bed reactor

IF 3.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
RSC Advances Pub Date : 2024-11-18 DOI:10.1039/D4RA06187J
Issara Sereewatthanawut, Notsawan Swadchaipong, Vut Tongnan, Chalempol Khajonvittayakul, Panupan Maneesard, Rossarin Ampairojanawong, Ammarika Makdee, Matthew Hartley, Kang Li and Unalome Wetwatana Hartley
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Abstract

A flower-like CeO2 catalyst was successfully synthesized using an acrylamide graft copolymerized on glucose under hydrothermal conditions and used for the direct synthesis of dimethyl carbonate (DMC) from CO2 and CH3OH in a packed-bed reactor with 2-cyanopyridine as a dehydrating agent. The synthesized flower-like CeO2 exhibited both basicity and acidity properties with values of 300 μmol g−1 and 80 μmol g−1, respectively, according to CO2-TPD and NH3-TPD results. The effect of reaction parameters such as reaction temperature, feed ratio, catalyst quantity, and operating pressure on the DMC production over the flower-like CeO2 catalyst was investigated. The optimum conditions were found to be a temperature of 120 °C, catalyst weight of 1.0 g, CH3OH : CO2 ratio of 1 : 1, and pressure of 30 bar, which provided the highest CH3OH conversion, DMC selectivity, and DMC yield of 86.6%, 99.3%, and 86.0%, respectively. Furthermore, no changes were observed in the structure, morphology, and particle size of the flower-like CeO2 catalyst after the DMC synthesis reaction, indicating that the synthesized catalyst was resistant to the reaction test under such optimum reaction conditions.

Abstract Image

在连续填料床反应器中,以 2-氰基吡啶为脱水剂,在花状 CeO2 催化剂上从二氧化碳和甲醇直接合成碳酸二甲酯
在水热条件下,利用丙烯酰胺在葡萄糖上的接枝共聚成功合成了一种花状 CeO2 催化剂,并将其用于在填料床反应器中以 2-氰基吡啶为脱水剂从 CO2 和 CH3OH 直接合成碳酸二甲酯(DMC)。根据 CO2-TPD 和 NH3-TPD 的结果,合成的花状 CeO2 同时具有碱性和酸性,其值分别为 300 μmol g-1 和 80 μmol g-1。研究了反应温度、进料比、催化剂用量和操作压力等反应参数对花状 CeO2 催化剂生产 DMC 的影响。研究发现,最佳条件为温度 120 °C、催化剂重量 1.0 克、CH3OH :二氧化碳的比例为 1 :1 : 1,压力为 30 巴,其 CH3OH 转化率、DMC 选择性和 DMC 收率最高,分别为 86.6%、99.3% 和 86.0%。此外,DMC 合成反应后,花状 CeO2 催化剂的结构、形貌和粒径均未发生变化,表明在这种最佳反应条件下,合成的催化剂能经受住反应的考验。
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来源期刊
RSC Advances
RSC Advances chemical sciences-
CiteScore
7.50
自引率
2.60%
发文量
3116
审稿时长
1.6 months
期刊介绍: An international, peer-reviewed journal covering all of the chemical sciences, including multidisciplinary and emerging areas. RSC Advances is a gold open access journal allowing researchers free access to research articles, and offering an affordable open access publishing option for authors around the world.
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