National Institute for Nanotechnology, National Research Council of Canada, 11421 Saskatchewan Drive, Edmonton, Alberta, Canada T6G 2M9.
Phys Chem Chem Phys. 2011 Feb 21;13(7):2780-7. doi: 10.1039/c0cp01537g. Epub 2010 Dec 14.
The interaction of CO(2) to the interior and exterior walls of pristine and nitrogen-doped single-walled carbon nanotubes (SWNT) has been studied using density-functional theory with dispersion-correcting potentials (DCPs). Our calculations predict Gibbs energies of binding between SWNT and CO(2) of up to 9.1 kcal mol(-1), with strongest binding observed for a zigzag [10,0] nanotube, compared to armchair [6,6] (8.3 kcal mol(-1)) and chiral [8,4] (7.0 kcal mol(-1)). Doping of the [10,0] tube with nitrogen increases the Gibbs energies of binding of CO(2) by ca. 3 kcal mol(-1), but slightly reduced binding is found when [6,6] and [8,4] SWNT are doped in similar fashion. The Gibbs energy of binding of CO(2) to the exterior of the tubes is quite small compared to the binding that occurs inside the tubes. These findings suggest that the zigzag SWNT show greater promise as a means of CO(2) gas-capture.
我们使用含弥散修正项的密度泛函理论研究了 CO(2)与原始和氮掺杂单壁碳纳米管（SWNT）内外壁的相互作用。我们的计算预测 SWNT 与 CO(2)之间的结合吉布斯自由能高达 9.1 kcal/mol(-1)，其中观察到最强的结合是锯齿形 [10,0] 纳米管，与扶手椅形 [6,6]（8.3 kcal/mol(-1)) 和手性 [8,4]（7.0 kcal/mol(-1)) 相比。氮掺杂 [10,0] 管会将 CO(2)的结合吉布斯自由能增加约 3 kcal/mol(-1)，但以类似方式掺杂 [6,6] 和 [8,4] SWNT 时，结合会略有减少。与管内发生的结合相比，CO(2)在管外的结合吉布斯自由能很小。这些发现表明，锯齿形 SWNT 作为 CO(2)气体捕获的手段具有更大的潜力。
