通过异环环膨胀环捕获酸性气体
Matthew P Confer1,2, David A Dixon2
1Beckman Institute for Advanced Science and Technology, University of Illinois Urbana-Champaign, Urbana, Illinois 61801, United States.
The journal of physical chemistry. A
|November 22, 2023
概括
研究人员通过计算方式研究了利用压力异常循环捕获二氧化碳 (CO2) 和二氧化硫 (SO2) 等酸性气体. 对于较小的环,环膨胀反应是外热的,为这些被捕获的气体提供了上循环的潜力.
科学领域:
- 计算化学的计算化学
- 绿色化学 绿色化学
- 材料科学 材料科学 材料科学
背景情况:
- 工业过程会排放酸性气体 (CO2,OCS,CS2,SO2),导致全球变暖和酸雨.
- 捕获和将这些酸性气体转化为有价值的产品是一个重大的技术挑战.
研究的目的:
- 通过使用应变异循环的环扩张计算调查CO2,CS2,SO2和OCS的捕获.
- 探索替代物 (,甲基,) 对异环中N和/或C原子的影响.
- 评估这些酸气捕获反应的热力学有利性和能量障碍.
主要方法:
- 密度函数理论 (DFT) 在G3级的计算.
- 研究涉及3个,4个和5个成员的应变异环的环膨胀反应.
- 替代物效应的分析和反应障碍与热力学的相关性.
主要成果:
- 捕获CO2,CS2,SO2和OCS的环膨胀反应对于3个和4个环是外热的,但对于5个环是不利的.
- CS2和OCS捕获反应比CO2和SO2捕获更外热,这是由于键解离的度差异.
- 反应能量障碍在二氧化碳和OCS捕获方面最高,在CS2和SO2捕获方面最低.
结论:
- 异循环通过环膨胀捕获酸气体的能力与环张力能量有关,但不仅仅取决于它.
- 由此产生的扩展N-异环显示出聚合的潜力,使得被捕获的酸性气体能够被循环转化为有用的材料.
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