Transferability of CO2 Force Fields for Prediction of Adsorption Properties in All-Silica Zeolites,The Journal of Physical Chemistry C

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Transferability of CO2 Force Fields for Prediction of Adsorption Properties in All-Silica Zeolites
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-04-19 00:00:00 , DOI: 10.1021/acs.jpcc.8b02208
Jian Ren Lim ₁ , Chi-Ta Yang ₁ , Jihan Kim ₂ , Li-Chiang Lin ₁

Affiliation

We present a systematic and comprehensive investigation of available CO₂ force fields for their predictions of adsorption properties in 156 geometrically diverse zeolite structures. The comparison reveals that a large discrepancy in the predicted properties, by more than 2 orders of magnitude, may exist. Especially, variation predicted by different force fields appears to be more pronounced for zeolites with more confined pore features, which can be attributed to the repulsive characteristics of force fields. The discrepancy especially impacts zeolites that are deemed to be the best materials for carbon capture and sequestration (CCS), indicating that the predictions on the best materials can drastically differ, based on the choice of force fields. To develop accurate and fully transferable force fields, in this work, we show that the inclusion of adsorption uptake at a high-pressure region (or saturation loading), as well as the diffusion coefficient, can be of utmost importance. These properties can be used as indicators for the repulsive behaviors between gas molecules and the framework. Mixture isotherms have also been identified to be potentially useful for the same purpose. Moreover, we have also demonstrated that interaction energies computed by ab initio methods can be useful references to ensure a newly developed force field is capable of describing the energy surface at an atomic level. Overall, the outcomes of this study will be instrumental to the future development of accurate and transferrable force fields, which is critical for future large-scale computational studies.

中文翻译：

CO ₂力场的传递性用于预测全硅沸石的吸附性能

我们对可用的CO ₂进行系统而全面的调查力场，以预测156种几何形状多样的沸石结构的吸附性能。比较表明，可能存在超过2个数量级的预测属性差异。特别是，对于孔隙特征更为局限的沸石，由不同力场预测的变化似乎更为明显，这可归因于力场的排斥特性。这种差异尤其会影响被认为是碳捕获和封存（CCS）最佳材料的沸石，这表明基于力场的选择，对最佳材料的预测可能会大不相同。为了开发精确且可完全转移的力场，在这项工作中，我们证明了在高压区域（或饱和载荷）下的吸收吸收包括在内，以及扩散系数，都是至关重要的。这些性质可以用作指示气体分子与框架之间排斥行为的指标。混合物等温线也已被确定对于同一目的可能有用。此外，我们还证明了从头算方法计算出的相互作用能可以作为确保新开发的力场能够描述原子级能表面的有用参考。总的来说，这项研究的结果将对未来精确和可传递力场的发展起重要作用，这对于未来的大规模计算研究至关重要。混合物等温线也已被确定对于同一目的可能有用。此外，我们还证明了从头算方法计算出的相互作用能可以作为确保新开发的力场能够描述原子级能表面的有用参考。总的来说，这项研究的结果将对未来精确和可传递力场的发展起重要作用，这对未来的大规模计算研究至关重要。混合物等温线也已被确定对于同一目的可能有用。此外，我们还证明了从头算方法计算出的相互作用能可以作为确保新开发的力场能够描述原子级能表面的有用参考。总的来说，这项研究的结果将对未来精确和可传递力场的发展起重要作用，这对于未来的大规模计算研究至关重要。

更新日期：2018-04-19

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