Bayesian Optimization-Assisted Engineering of Formate Dehydrogenase Encapsulation in Multivariate Zeolitic Imidazolate Framework

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2024-12-19 DOI:10.1021/acs.chemmater.4c02816

Weibin Liang, Sisi Zheng, Ying Shu, Jun Huang

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Abstract

Engineering of multivariate zeolitic imidazolate frameworks (mZIFs) offers substantial potential for optimizing enzyme encapsulation by enhancing encapsulation efficiency (EE), enzyme loading capacity (P_loading), retained enzymatic activity (REA), and protection. However, this area remains underexplored. In this study, we rationally employed three imidazole-based ligands with distinct functionalities─HeIM (2-ethylimidazole), HTz (1,2,4-triazole), and HIM (1-(2-hydroxyethyl)imidazole)─to fine-tune hydrophobicity and defect simultaneously within FDH@mZIF (FDH = formate dehydrogenase). Leveraging an iterative Bayesian optimization-assisted training-design-synthesis-measurement workflow, we efficiently identified F190 as the best FDH@mZIF, achieving EE = 89.3%, REA = 14.9%, and P_loading = 30.3 wt%. This establishes F190 as the leading FDH-based biocatalyst in the literature. The optimal FDH-mZIF interactions in F190 were reflected by minimal structural perturbation of encapsulated FDH, as evidenced by the ATR-FTIR and fluorescence studies. Additionally, F190 can effectively safeguard the encapsulated FDH against thermal and proteolytic degradation and catalyze CO₂-to-formate conversion while maintaining activity for at least five cycles without significant activity loss.

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通过提高封装效率（EE）、酶装载能力（Ploading）、酶活性保持率（REA）和保护能力，多元沸石咪唑框架（mZIFs）工程技术为优化酶封装提供了巨大的潜力。然而，这一领域仍未得到充分探索。在本研究中，我们合理地使用了三种具有不同功能性的咪唑类配体--HeIM（2-乙基咪唑）、HTz（1,2,4-三唑）和 HIM（1-(2-羟乙基)咪唑）--来同时微调 FDH@mZIF （FDH = 甲酸脱氢酶）的疏水性和缺陷。利用贝叶斯迭代优化辅助训练-设计-合成-测量工作流程，我们有效地确定了 F190 为最佳 FDH@mZIF，其 EE = 89.3%、REA = 14.9%、Ploading = 30.3 wt%。这使得 F190 成为文献中基于 FDH 的领先生物催化剂。ATR-FTIR 和荧光研究表明，封装 FDH 的结构扰动极小，这反映了 F190 中 FDH 与 ZIF 之间的最佳相互作用。此外，F190 还能有效保护封装的 FDH 免受热降解和蛋白酶降解的影响，并能催化 CO2 到甲酸的转化，同时在至少五个循环中保持活性而不会出现明显的活性损失。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.