Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia.
Phys Chem Chem Phys. 2011 Aug 7;13(29):13410-20. doi: 10.1039/c0cp02702b. Epub 2011 Jun 28.
A new predictive computational method for classifying clathrate hydrate promoter molecules is presented, based on the interaction energies between potential promoters and the water networks of sII and sH clathrates. The motivation for this work is identifying promoters for storing hydrogen compactly in clathrate hydrates. As a first step towards achieving this goal, we have developed a general method aimed at distinguishing between molecules that form sII clathrate hydrates and molecules that can-together with a weakly interacting help gas-form sH clathrate hydrates. The new computational method calculates differences in estimated formation energies of the sII and the sH clathrate hydrate. Model interaction potentials have been used, including the electrostatic interactions with newly calculated partial charges for all the considered potential promoter molecules. The methodology can discriminate between the clathrate structure types (sII or sH) formed by each potential promoter with good selectivity, i.e., better than achieved with a simple van der Waals diameter criterion.
提出了一种新的预测计算方法，用于根据潜在促进剂与 sII 和 sH 笼形水合物的水网络之间的相互作用能对笼形水合物促进剂分子进行分类。这项工作的动机是确定在笼形水合物中储存氢气的促进剂。作为实现这一目标的第一步，我们开发了一种通用方法，旨在区分形成 sII 笼形水合物的分子和可以与弱相互作用的助气一起形成 sH 笼形水合物的分子。新的计算方法计算了 sII 和 sH 笼形水合物的估计形成能的差异。使用了模型相互作用势能，包括对所有考虑的潜在促进剂分子的新计算的部分电荷的静电相互作用。该方法可以很好地区分每个潜在促进剂形成的笼形结构类型（sII 或 sH），即选择性优于简单的范德华直径标准。
