Pyrene-based ammonium bromides combined with g-C(3)N(4) for the synergistically enhanced fixation reaction of CO(2) and epoxides.

Pyrene-based ammonium bromides combined with g-C(3)N(4) for the synergistically enhanced fixation reaction of CO(2) and epoxides.
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芘基溴化铵与 g-C3N4 结合,协同增强 CO2 和环氧化物的固定反应

DOI:
10.1039/d1ra05328k
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发表时间:
2021-09-06
期刊:
影响因子:
3.9
通讯作者:
--
中科院分区:
化学3区
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通过溴甲基芘和不同烷基链的叔胺与石墨氮化碳(g-C3N4)通过π-π堆积相互作用反应,合成了一种新型芘基溴化铵(PABs)。研究了新型芘基溴化铵在均相和异相中与 g-C3N4 的结合,在温和条件下进行环氧化物的 CO2 固定反应。显然,该组合被证明是环氧化物转化的有效系统。 g-C3N4 和 PAB 之间的相互作用通过量子化学计算得到证实。 g-C3N4/Py-C12在80℃、大气压和无溶剂条件下表现出优异的环状碳酸酯产率(高于93%)。使用 g-C3N4/Py-C12 进行初步动力学研究,计算出活化能为 61.5 kJ mol−1。 g-C3N4 和 PAB 的协同相互作用在环氧化物的 CO2 固定反应中发挥着重要作用。
A new type of pyrene-based ammonium bromides (PABs) was synthesized via the reaction of bromomethyl pyrene and tertiary amines with different alkyl chains combined with graphitic carbon nitride (g-C3N4) through π–π stacking interactions. The new pyrene-based ammonium bromides were investigated both in homogenous phase and heterogeneous phase combining with g-C3N4 for the CO2 fixation reaction of epoxides under mild conditions. Obviously, the combination was proved to be an efficient system for the conversion of epoxides. The interaction between g-C3N4 and PABs was confirmed by quantum chemical calculations. g-C3N4/Py-C12 exhibited an excellent yield of cyclic carbonates (above 93%) at 80 °C, atmospheric pressure and solvent-free conditions. A preliminary kinetic study was performed using g-C3N4/Py-C12 and the activation energy was calculated to be 61.5 kJ mol−1. The synergistic interaction of g-C3N4 and PABs plays an important role in the CO2 fixation reaction with epoxides.
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