Theoretical studies of carbon-centered organocatalysts for CO2 activation and mechanism studies for its conversion to methanol are the purposes of this research. Three possible pathways are proposed in this study for methanol production from CO2 and 9-BBN. Two distinct mechanisms can be considered for CO2 activation, which include an insertion reaction and a two-step reaction. The activation strain model (ASM) and electron localization function (ELF) concepts were applied for justification of the nucleophilic attack behavior of the studied organocatalysts in CO2 activation. Proton transfer in step 2 of the CO2 activation is studied as the rate-determining step of the reaction by nuclear-independent chemical shift (NICS-XY) scan. The results show that a lower absolute value of NICSnZZ in the case of organocatalysts with an electron-withdrawing group represents a higher stabilization in developing π-electron on the five-member ring of the organocatalysts and a lower ∆G≠ value than the other ones. Finally, the organocatalysts with the electron withdrawing substituents are kinetically and thermodynamically the best candidates for CO2 activation based on various different analyses.

中文翻译：

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两性离子茚基铵衍生物作为一类新型碳中心有机催化剂将 CO2 转化为甲醇的性能研究

用于 CO2 活化的碳中心有机催化剂的理论研究及其转化为甲醇的机制研究是本研究的目的。本研究提出了从 CO2 和 9-BBN 生产甲醇的三种可能途径。可以考虑两种不同的 CO2 活化机制，包括插入反应和两步反应。活化应变模型 (ASM) 和电子定位函数 (ELF) 概念用于证明所研究的有机催化剂在 CO2 活化中的亲核攻击行为的合理性。通过与核无关的化学位移 (NICS-XY) 扫描，将 CO2 活化步骤 2 中的质子转移作为反应的速率决定步骤进行研究。结果表明，在具有吸电子基团的有机催化剂的情况下，NICSnZZ 的绝对值较低表示在有机催化剂的五元环上发展 π 电子的稳定性更高，ΔG≠ 值低于其他有机催化剂. 最后，基于各种不同的分析，具有吸电子取代基的有机催化剂在动力学和热力学上是 CO2 活化的最佳候选者。