探索二氧化碳的乙烯氧化物的替代策略 封存和催化转换:理论研究
Lina Yin1, Renjie Zhou1, Yiping Lv1
1College of Chemistry and Materials Science, Jinan University, 601 Huang-Pu Avenue West, Guangzhou 510632, China.
ACS omega
|December 11, 2023
概括
将氨基组附着在乙烯氧化物上显著降低了CO2循环添加障碍,从而使CO2固定更温和. 这一发现有助于利用催化剂有效地将二氧化碳转化为有价值的化学物质.
科学领域:
- 计算化学的计算化学
- 材料科学 材料科学 材料科学
- 绿色化学 绿色化学
背景情况:
- 乙烯氧化物是一种关键的工业化学品.
- 二氧化碳 (CO2) 的利用仍然是绿色化学的一个重大挑战.
- 目前正在积极研究二氧化碳循环添加的催化和非催化方法.
研究的目的:
- 为了研究氨基替代剂对二氧化碳循环添加的乙烯氧化物的作用.
- 阐明减少反应屏障背后的机制.
- 探索改性乙烯氧化物在二氧化碳固定和转化中的潜力.
主要方法:
- 密度函数理论 (DFT) 的计算.
- 分析局部电荷,边界轨道和电子转移.
- 扭曲/相互作用激活应变模型 (D/I-ASM) 模拟.
主要成果:
- 氨基基替代乙烯氧化物,特别是 -N(CH3) 2-单替代乙烯氧化物 (NEO),极大地降低了CO2循环添加障碍,从69.5到22.1kcal/mol.
- 屏障高度的降低归因于激活应变的降低和分子间相互作用的增加.
- NEO促进了二氧化碳的封存和随后的转化为二甲基碳酸盐和N,N'-二甲基尿素与催化剂,如TBD.
结论:
- 乙烯氧化物的氨基功能化为在温和条件下有效的二氧化碳捕获和利用提供了一个有希望的途径.
- NEO作为有效的二氧化碳固定和转化基质,可能适用于环氧树脂.
- 这项研究为将氨基功能纳入环氧化物为可持续化学合成铺平了道路.
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