JACS Au Pub Date : 2024-08-12 DOI: 10.1021/jacsau.4c00488

Yizhen Wang, Zihan Lin, Runhai Ouyang, Bin Jiang, Igor Ying Zhang, Xin Xu

{"title":"Toward Efficient and Unified Treatment of Static and Dynamic Correlations in Generalized Kohn–Sham Density Functional Theory","authors":"Yizhen Wang, Zihan Lin, Runhai Ouyang, Bin Jiang, Igor Ying Zhang, Xin Xu","doi":"10.1021/jacsau.4c00488","DOIUrl":"https://doi.org/10.1021/jacsau.4c00488","url":null,"abstract":"Accurate description of the static correlation poses a persistent challenge in electronic structure theory, particularly when it has to be concurrently considered with the dynamic correlation. We develop here a method in the generalized Kohn–Sham density functional theory (DFT) framework, named R-xDH7-SCC15, which achieves an unprecedented accuracy in capturing the static correlation, while maintaining a good description of the dynamic correlation on par with the state-of-the-art DFT and wave function theory methods, all grounded in the same single-reference black-box methodology. Central to R-xDH7-SCC15 is a general-purpose static correlation correction (SCC) model applied to the renormalized XYG3-type doubly hybrid method (R-xDH7). The SCC model development involves a hybrid machine learning strategy that integrates symbolic regression with nonlinear parameter optimization, aiming to achieve a balance between generalization capability, numerical accuracy, and interpretability. Extensive benchmark studies confirm the robustness and broad applicability of R-xDH7-SCC15 across a diverse array of main-group chemical scenarios. Notably, it displays exceptional aptitude in accurately characterizing intricate reaction kinetics and dynamic processes in regions distant from equilibrium, where the influence of static correlation is most profound. Its capability to consistently and efficiently predict the whole energy profiles, activation barriers, and reaction pathways within a user-friendly “black-box” framework represents an important advance in the field of electronic structure theory.","PeriodicalId":14799,"journal":{"name":"JACS Au","volume":"20 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141969510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Machine Learning Optimizing Enzyme/ZIF Biocomposites for Enhanced Encapsulation Efficiency and Bioactivity 机器学习优化酶/ZIF 生物复合材料，提高封装效率和生物活性

JACS Au Pub Date : 2024-08-12 DOI: 10.1021/jacsau.4c00485

Weibin Liang, Sisi Zheng, Ying Shu, Jun Huang

{"title":"Machine Learning Optimizing Enzyme/ZIF Biocomposites for Enhanced Encapsulation Efficiency and Bioactivity","authors":"Weibin Liang, Sisi Zheng, Ying Shu, Jun Huang","doi":"10.1021/jacsau.4c00485","DOIUrl":"https://doi.org/10.1021/jacsau.4c00485","url":null,"abstract":"In this study, we present the first example of using a machine learning (ML)-assisted design strategy to optimize the synthesis formulation of enzyme/ZIFs (zeolitic imidazolate framework) for enhanced performance. Glucose oxidase (GOx) and horseradish peroxidase (HRP) were chosen as model enzymes, while Zn(eIM)2 (eIM = 2-ethylimidazolate) was selected as the model ZIF to test our ML-assisted workflow paradigm. Through an iterative ML-driven training-design-synthesis-measurement workflow, we efficiently discovered GOx/ZIF (G151) and HRP/ZIF (H150) with their overall performance index (OPI) values (OPI represents the product of encapsulation efficiency (E in %), retained enzymatic activity (A in %), and thermal stability (T in %)) at least 1.3 times higher than those in systematic seed data studies. Furthermore, advanced statistical methods derived from the trained random forest model qualitatively and quantitatively reveal the relationship among synthesis, structure, and performance in the enzyme/ZIF system, offering valuable guidance for future studies on enzyme/ZIFs. Overall, our proposed ML-assisted design strategy holds promise for accelerating the development of enzyme/ZIFs and other enzyme immobilization systems for biocatalysis applications and beyond, including drug delivery and sensing, among others.","PeriodicalId":14799,"journal":{"name":"JACS Au","volume":"31 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141946203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Spectroscopic Characterization of the 1-Boratricyclo-[4.1.0.02,7]-heptane Radical with a Delocalized Four-Center-One-Electron Bond 具有去局域化四中心一电子键的 1-硼杂三环-[4.1.0.02,7]庚烷自由基的光谱特征

JACS Au Pub Date : 2024-08-09 DOI: 10.1021/jacsau.4c00492

Chuan-Ming Dai, Jiaping Xu, Xin Xu, Cong Wang, Tao You, Wei Li, Jiwen Jian

引用次数: 0

An Enzymatic Oxidation Cascade Converts δ-Thiolactone Anthracene to Anthraquinone in the Biosynthesis of Anthraquinone-Fused Enediynes 在蒽醌-融合烯二炔的生物合成过程中，δ-硫内酯蒽向蒽醌的酶促氧化级联转化

JACS Au Pub Date : 2024-08-09 DOI: 10.1021/jacsau.4c00279

Guang-Lei Ma, Wanqiu Liu, Huawei Huang, Xin-Fu Yan, Wei Shen, Surawit Visitsatthawong, Kridsadakorn Prakinee, Hoa Tran, Xiaohui Fan, Yong‐Gui Gao, P. Chaiyen, Jian Li, Zhao-Xun Liang

引用次数: 0

An Aptamer Glue Enables Hyperefficient Targeted Membrane Protein Degradation 一种能实现高效定向膜蛋白降解的 Aptamer 胶水

JACS Au Pub Date : 2024-08-08 DOI: 10.1021/jacsau.4c00260

Guo-Rong Zhang, Chi Zhang, Ting Fu, Weihong Tan, Xueqiang Wang

引用次数: 0

Challenges and Future Perspectives in Photocatalysis: Conclusions from an Interdisciplinary Workshop 光催化技术的挑战与未来展望：跨学科研讨会的结论

JACS Au Pub Date : 2024-08-08 DOI: 10.1021/jacsau.4c00527

Sebastian B. Beil, Sylvestre Bonnet, Carla Casadevall, R. Detz, Fabian Eisenreich, Starla D. Glover, Christoph Kerzig, Line Næsborg, Sonja Pullen, Golo Storch, Ning Wei, Cathleen Zeymer

引用次数: 0

Structure-Based Design of CBP/EP300 Degraders: When Cooperativity Overcomes Affinity 基于结构设计的 CBP/EP300 降解剂：当合作性战胜亲和性时

JACS Au Pub Date : 2024-08-08 DOI: 10.1021/jacsau.4c00292

Iván Cheng-Sánchez, Katherine A. Gosselé, Leonardo Palaferri, E. Laul, Gionata Riccabella, R. K. Bedi, Yaozong Li, Anna Müller, Ivan Corbeski, A. Caflisch, Cristina Nevado

引用次数: 0

Engineering Central Substitutions in Heptamethine Dyes for Improved Fluorophore Performance 在七甲基染料中进行中心取代工程以提高发荧光体的性能

JACS Au Pub Date : 2024-08-07 DOI: 10.1021/jacsau.4c00343

Lei Guo, Meek Yang, Bin Dong, Seth Lewman, Alex Van Horn, Shang Jia

{"title":"Engineering Central Substitutions in Heptamethine Dyes for Improved Fluorophore Performance","authors":"Lei Guo, Meek Yang, Bin Dong, Seth Lewman, Alex Van Horn, Shang Jia","doi":"10.1021/jacsau.4c00343","DOIUrl":"https://doi.org/10.1021/jacsau.4c00343","url":null,"abstract":"As a major family of red-shifted fluorophores that operate beyond visible light, polymethine dyes are pivotal in light-based biological techniques. However, methods for tuning this kind of fluorophores by structural modification remain restricted to bottom-up synthesis and modification using coupling or nucleophilic substitutions. In this study, we introduce a two-step, late-stage functionalization process for heptamethine dyes. This process enables the substitution of the central chlorine atom in the commonly used 4′-chloro heptamethine scaffold with various aryl groups using aryllithium reagents. This method borrows the building block and designs from the xanthene dye community and offers a mild and convenient way for the diversification of heptamethine fluorophores. Notably, this efficient conversion allows for the synthesis of heptamethine-X, the heptamethine scaffold with two ortho-substituents on the 4′-aryl modification, which brings enhanced stability and reduced aggregation to the fluorophore. We showcase the utility of this method by a facile synthesis of a fluorogenic, membrane-localizing fluorophore that outperforms its commercial counterparts with a significantly higher brightness and contrast. Overall, this method establishes the synthetic similarities between polymethine and xanthene fluorophores and provides a versatile and feasible toolbox for future optimizing heptamethine fluorophores for their biological applications.","PeriodicalId":14799,"journal":{"name":"JACS Au","volume":"11 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141946204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Temperature Effects and Activation Barriers in Aqueous Proton-Uptake Reactions 水质质子吸收反应中的温度效应和活化障碍

JACS Au Pub Date : 2024-08-06 DOI: 10.1021/jacsau.4c00326

Balázs Antalicz, Huib J. Bakker

引用次数: 0

Transition-Metal-Free C-Diarylations to Reach All-Carbon Quaternary Centers 通过无过渡金属 C-二芳基化达到全碳季态中心

JACS Au Pub Date : 2024-08-05 DOI: 10.1021/jacsau.4c00500

Shobhan Mondal, Benjamin Gunschera, Berit Olofsson

引用次数: 0

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