贝叶斯优化
公制(单位)
相似性(几何)
功能(生物学)
现存分类群
计算机科学
贝叶斯概率
空格(标点符号)
核(代数)
化学空间
金属有机骨架
吸附
数学
化学
人工智能
工程类
生物
有机化学
操作系统
图像(数学)
组合数学
进化生物学
药物发现
生物化学
运营管理
作者
Tsung-Wei Liu,Quan Nguyen,Adji B. Dieng,Diego A. Gómez‐Gualdrón
标识
DOI:10.26434/chemrxiv-2024-fqll9
摘要
Metal-organic frameworks (MOFs) promise to engender technology-enabling properties for numerous applications. However, one significant challenge in MOF development is their overwhelmingly large design space, which is intractable to fully explore even computationally. To find diverse optimal MOF designs without exploring the full design space, we develop Vendi Bayesian optimization (VBO), a new algorithm that combines traditional Bayesian optimization with the Vendi Score, a recently introduced interpretable diversity measure. Both Bayesian optimization and the Vendi Score require a kernel similarity function, we therefore also introduce a novel similarity function in the space of MOFs that accounts for both chemical and structural features. This new similarity metric enables VBO to find optimal MOFs with properties that may depend on both chemistry and structure. We statistically assessed VBO by its ability to optimize three NH3-adsorption dependent performance metrics that depend, to different degrees, on MOF chemistry and structure. With ten simulated campaigns done for each metric, VBO consistently outperformed random search to find high-performing designs within a 1,000-MOF subset for i) NH3 storage, ii) NH3 removal from membrane plasma reactors, and iii) NH3 capture from air. Then, with one campaign dedicated to finding optimal MOFs for NH3 storage in a “hybrid” ~10,000-MOF database, we identify twelve extant and eight hypothesized MOF designs with potentially record-breaking working capacity ∆NNH3 between 300 K and 400 K at 1 bar. Specifically, the best MOF designs are predicted to i) achieve ∆NNH3 values between 23.6 and 29.3 mmol/gm, potentially surpassing those that MOFs previously experimentally tested for NH3 adsorption would have at the proposed operation conditions, ii) be thermally stable at the operation conditions and iii) require only ca. 10% of the energy content in NH3 to release the stored molecule from the MOF. Finally, the analysis of the generated simulation data during the search indicates that a pore size of around 10 Å, a heat of adsorption around 33 kJ/mol, and the presence of Ca could be part of MOF design rules that could help optimize NH3 working capacity at the proposed operation conditions
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