当前位置：
X-MOL 学术
›
J. Phys. Chem. A
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Accurate Thermochemical and Kinetic Stabilities of C84 Isomers
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-04-24 00:00:00 , DOI: 10.1021/acs.jpca.8b02404 Simone L. Waite 1 , Bun Chan 2 , Amir Karton 3 , Alister J. Page 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-04-24 00:00:00 , DOI: 10.1021/acs.jpca.8b02404 Simone L. Waite 1 , Bun Chan 2 , Amir Karton 3 , Alister J. Page 1
Affiliation
|
Accurate double-hybrid density functional theory and isodesmic-type reaction schemes are utilized to report accurate estimates of the heats of formation (ΔfH) for all 24 isolated-pentagon-rule isomers of the third most abundant fullerene, C84. Kinetic stabilities of these C84 isomers are also considered via C–C bond cleavage rates (Pcleav) calculated using density functional theory. Our results show that the relative abundance of C84 fullerene isomers observed in arc discharge synthesis is the result of both thermochemical and kinetic factors. This provides timely insight regarding the characterization of several C84 isomers that have been obtained experimentally to date. For instance, the established assignments of C84 isomers of (using the Fowler–Manolopoulos numbering scheme) 22 [D2(IV)], 23 [D2d(II)], 19 [D3d], 24 [D6h], 11 [C2(IV)], and 4 [D2d(I)] are consistent with the relative ΔfH and Pcleav values for these structures. However, our thermochemical and kinetic stabilities of Cs isomers 14, 15, and 16 indicate that the two experimentally isolated Cs isomers are 15 and 16, contrary to some previous assignments. Of the remaining isolated isomers of symmetry C2 and D2, definitive assignment was not possible with consideration of only ΔfH and Pcleav.
中文翻译：
C 84异构体的准确热化学和动力学稳定性
准确的双杂化密度泛函理论和等渗型反应方案可用于报告第三富勒烯C 84的所有24种分离的五边形规则异构体的形成热（Δf H）的准确估算。这些C 84异构体的动力学稳定性也可以通过使用密度泛函理论计算的C–C键断裂速率（P cleav）来考虑。我们的结果表明，在电弧放电合成中观察到的C 84富勒烯异构体的相对丰度是热化学和动力学因素共同作用的结果。这提供了有关几种C 84的表征的及时见解迄今为止已通过实验获得的异构体。例如，已确定的C 84异构体的分配（使用Fowler-Manolopoulos编号方案）22 [ D 2（IV）]，23 [ D 2 d（II）]，19 [ D 3 d ]，24 [ D 6 h ]，11 [ C 2（IV）]和4 [ D 2 d（I）]与这些结构的相对Δf H和P cleav值一致。然而，我们的热化学和动力学稳定性Ç小号异构体14、15和16表明两个实验分离的C s异构体分别为15和16，这与某些先前的定义相反。在其余的对称的C 2和D 2分离异构体中，仅考虑Δf H和P cleav不可能确定分配。
更新日期：2018-04-24
中文翻译：
C 84异构体的准确热化学和动力学稳定性
准确的双杂化密度泛函理论和等渗型反应方案可用于报告第三富勒烯C 84的所有24种分离的五边形规则异构体的形成热（Δf H）的准确估算。这些C 84异构体的动力学稳定性也可以通过使用密度泛函理论计算的C–C键断裂速率（P cleav）来考虑。我们的结果表明，在电弧放电合成中观察到的C 84富勒烯异构体的相对丰度是热化学和动力学因素共同作用的结果。这提供了有关几种C 84的表征的及时见解迄今为止已通过实验获得的异构体。例如，已确定的C 84异构体的分配（使用Fowler-Manolopoulos编号方案）22 [ D 2（IV）]，23 [ D 2 d（II）]，19 [ D 3 d ]，24 [ D 6 h ]，11 [ C 2（IV）]和4 [ D 2 d（I）]与这些结构的相对Δf H和P cleav值一致。然而，我们的热化学和动力学稳定性Ç小号异构体14、15和16表明两个实验分离的C s异构体分别为15和16，这与某些先前的定义相反。在其余的对称的C 2和D 2分离异构体中，仅考虑Δf H和P cleav不可能确定分配。
京公网安备 11010802027423号