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Methods for synthesizing diethyl carbonate from ethanol and supercritical carbon dioxide by one-pot or two-step reactions in the presence of potassium carbonate

机译:在碳酸钾存在下通过一锅或两步反应由乙醇和超临界二氧化碳合成碳酸二乙酯的方法

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摘要

Carbon dioxide sequestration was studied by synthesizing diethyl carbonate (DEC) from ethanol and CO2 under supercritical conditions in the presence of potassium carbonate as a base. The co-reagent was ethyl iodide or a concentrated strong acid. This sequestration reaction occurs in two steps, which were studied separately and in a one-pot reaction. An organic-inorganic carbonate hybrid, potassium ethyl carbonate (PEC) is generated at the end of the first step. This intermediate was characterized and was found to be a target molecule for CO2 capture. Different co-reactants, such as ethyl iodide and concentrated strong Brönsted acid, were compared in the second step and used to investigate the reactivity of the hybrid. With ethyl iodide as the co-reactant, one-pot DEC synthesis gave higher yields (46%) than two-step production. The supercritical CO2 acts as a swelling solvent and compatibilizing agent in the reaction medium, favoring interactions between ethanol and CO2 and between PEC and ethyl iodide. The use of a phase transfer catalyst (PTC) increased DEC production (yield 51%) without increasing the amount of diethyl ether (DEE) produced as a by-product (yield 2%).
机译:通过在碳酸钾为碱的超临界条件下由乙醇和二氧化碳合成碳酸二乙酯(DEC)来研究二氧化碳的固存。辅助试剂是碘乙烷或浓强酸。螯合反应分两个步骤进行,分别进行了研究,并在一个反应​​釜中进行。在第一步结束时,生成了有机-无机碳酸酯杂化物碳酸乙基钾(PEC)。对该中间体进行了表征,发现该中间体是捕获CO2的目标分子。在第二步中比较了不同的共反应物,如乙基碘和浓布朗斯台德酸,并用于研究杂化体的反应性。用碘乙烷作助反应剂,一锅法DEC合成比两步法生产的产率高(46%)。超临界CO2在反应介质中充当溶胀剂和增容剂,促进乙醇与CO2之间以及PEC与乙基碘之间的相互作用。使用相转移催化剂(PTC)可以增加DEC的产量(产率51%),而不会增加副产物二乙醚(DEE)的产量(产率2%)。

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