Department of Chemistry, University of Crete, Heraklion 71003, Greece.
J Chem Inf Model. 2024 Nov 11;64(21):8193-8200. doi: 10.1021/acs.jcim.4c01298. Epub 2024 Oct 31.
In the past decade, high-throughput computational studies of materials have increased significantly mainly due to advances in computer capabilities and have attracted a great deal of interest. In the field of metal-organic frameworks (MOFs), over a million hypothetical MOFs have been designed in silico, yet only a small fraction of these have been synthesized. For validating the computational-hypothetical results and accelerating the progress in the field, there is a pressing need for distinguishing MOFs that are more likely to be synthesized for real-life applications. This study presents a comprehensive investigation into the synthesizability likelihood of MOFs, utilizing a novel computational approach based on the disparities in energy and geometry between the linker conformation within the MOF structure and its isolated, free-gas state since both of these have been proven to be critical factors influencing MOF synthesis. Our user-friendly tool streamlines synthesizability evaluation, requiring minimal expertise in computational chemistry. By deconstructing over 40,000 MOFs from databases, including QMOF, CoRE MOF, and ToBaCCo, we analyze key parameters defining the linker strain within the MOF unit cell. Our results indicate that QMOF and CoRE MOF contain more promising candidates for synthesis, while ToBaCCo exhibits a relatively poor synthesizability likelihood due to unoptimized materials. Through extensive analysis, we identify optimal linker candidates for highly synthesizable MOFs. Consistent trends in energy distribution across databases that are confirmed by high Pearson and Spearman coefficients suggest the potential for omitting optimization calculations, significantly reducing computational costs. This study underscores the importance of linker deformation and energy disparities and enhances our understanding of synthetic accessibility in MOF research, offering valuable insights for future advancements in the field.
在过去的十年中，由于计算机能力的进步，高通量计算材料研究显著增加，并引起了极大的兴趣。在金属有机骨架（MOFs）领域，已经在计算机中设计了超过一百万种假设的 MOFs，但只有一小部分得到了合成。为了验证计算假设的结果并加速该领域的进展，迫切需要区分更有可能用于实际应用的 MOFs。本研究利用一种新颖的计算方法，对 MOFs 的可合成性进行了全面研究，该方法基于 MOF 结构内配体构象与其游离、自由气体状态之间的能量和几何差异，因为这两者都已被证明是影响 MOF 合成的关键因素。我们的用户友好型工具简化了可合成性评估，只需对计算化学有最低限度的专业知识。通过对来自 QMOF、CoRE MOF 和 ToBaCCo 等数据库的超过 40000 个 MOFs 进行解构，我们分析了定义 MOF 单元内配体应变的关键参数。我们的结果表明，QMOF 和 CoRE MOF 包含更有前途的合成候选物，而 ToBaCCo 由于材料未优化，其可合成性较低。通过广泛的分析，我们为高度可合成的 MOFs 确定了最佳的配体候选物。跨数据库的能量分布趋势一致，皮尔逊和斯皮尔曼系数较高，这表明可以省略优化计算，从而显著降低计算成本。本研究强调了配体变形和能量差异的重要性，并提高了我们对 MOF 研究中合成可及性的理解，为该领域的未来发展提供了有价值的见解。
