Incorporating Flexibility Effects into Metal–Organic Framework Adsorption Simulations Using Different Models,ACS Applied Materials & Interfaces

当前位置： X-MOL 学术 › ACS Appl. Mater. Interfaces › 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.)

Incorporating Flexibility Effects into Metal–Organic Framework Adsorption Simulations Using Different Models
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-12-20 , DOI: 10.1021/acsami.1c20583
Zhenzi Yu ₁ , Dylan M Anstine _{2,

3} , Salah Eddine Boulfelfel ₁ , Chenkai Gu _{1,

4,

5} , Coray M Colina _{2,

3,

6} , David S Sholl _{1,

7}

Affiliation

High-throughput calculations based on molecular simulations to predict the adsorption of molecules inside metal–organic frameworks (MOFs) have become a useful complement to experimental efforts to identify promising adsorbents for chemical separations and storage. For computational convenience, all existing efforts of this kind have relied on simulations in which the MOF is approximated as rigid. In this paper, we use extensive adsorption–relaxation simulations that fully include MOF flexibility effects to explore the validity of the rigid framework approximation. We also examine the accuracy of several approximate methods to incorporate framework flexibility that are more computationally efficient than adsorption–relaxation calculations. We first benchmark various models of MOF flexibility for four MOFs with well-established CO₂ experimental consensus isotherms. We then consider a range of adsorption properties, including Henry’s constants, nondilute loadings, and adsorption selectivity, for seven adsorbates in 15 MOFs randomly selected from the CoRE MOF database. Our results indicate that in many MOFs adsorption–relaxation simulations are necessary to make quantitative predictions of adsorption, particularly for adsorption at dilute concentrations, although more standard calculations based on rigid structures can provide useful information. Finally, we investigate whether a correlation exists between the elastic properties of empty MOFs and the importance of including framework flexibility in making accurate predictions of molecular adsorption. Our results did not identify a simple correlation of this type.

中文翻译：

使用不同模型将灵活性效应纳入金属-有机框架吸附模拟

基于分子模拟的高通量计算来预测分子在金属有机框架 (MOF) 内的吸附，已成为对实验工作的有用补充，以确定用于化学分离和储存的有前途的吸附剂。为了计算方便，所有现有的此类努力都依赖于模拟，其中 MOF 近似为刚性。在本文中，我们使用完全包含 MOF 柔性效应的广泛吸附-松弛模拟来探索刚性框架近似的有效性。我们还检查了几种近似方法的准确性，以结合框架灵活性，这些方法在计算上比吸附-弛豫计算更有效。我们首先对具有完善的 CO 的四个 MOF 的各种 MOF 灵活性模型进行了基准测试₂实验一致等温线。然后，我们考虑了一系列吸附特性，包括亨利常数、非稀释负载和吸附选择性，对于从 CoRE MOF 数据库中随机选择的 15 个 MOF 中的七种吸附物。我们的结果表明，在许多 MOF 中，吸附-弛豫模拟对于定量预测吸附是必要的，特别是对于稀释浓度下的吸附，尽管基于刚性结构的更多标准计算可以提供有用的信息。最后，我们研究了空 MOF 的弹性特性与包括框架灵活性在准确预测分子吸附方面的重要性之间是否存在相关性。我们的结果没有确定这种类型的简单相关性。

更新日期：2021-12-29

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南