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Divergent Protein Engineering of Transaminase for the Synthesis of Chiral Rivastigmine and Apremilast Precursors

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Chinese Journal of Chemistry 2024年第19期42卷 2335-2340页

作者： Langyu Tang Xinjie Yang Ningning Sun Guojiao wu yuzhou wu Fangrui Zhong Hubei Engineering Research Center for Biomaterials and Medical Protective Materials Hubei Key Laboratory of Bioinorganic Chemistry&Materia MedicaSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology1037 Luoyu RoadWuhanHubei 430074China Longgang Institute of Zhejiang Sci-Tech University WenzhouZhejiang 325802China Shenzhen Huazhong University of Science and Technology Research Institute ShenzhenGuangdong 518000China

Comprehensive Summary The implementation of divergent protein engineering on the natural transaminase Vf-ω-TA led to the development of two effective mutants(M2 and M8),enabling the enzymatic synthesis of chiral amine precursors of Rivastigmine and Apremilast,*** evolution of the enzymes was guided by crystal structures and a focused mutagenesis strategy,allowing them to effectively address the challenging ketone substrates with significant steric *** the optimized reaction parameters,transamination proceeded smoothly in good conversions and with perfect stereochemical control(>99%ee).These processes utilize inexpensiveα-methylbenzylamine as an amine donor and avoid the continuous acetone removal and costly LDH/GDH/NADH systems.

关键词： Asymmetric catalysis Chiral amine Protein engineering Directed evolution Biocatalysis Transaminase Enantioselectivity Syntheticmethods Amination Enzymes

Polymer coated nanodiamonds as gemcitabine prodrug with enzymatic sensitivity for pancreatic cancer treatment

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Progress in Natural Science:Materials International 2020年第5期30卷 711-717页

作者： Wanying Ye Haijie Han Huan Li Qiao Jin yuzhou wu Sabyasachi Chakrabortty Tanja Weil Jian Ji MOE Key Laboratory of Macromolecule Synthesis and Functionalization of Ministry of Education Department of Polymer Science and Engineering Zhejiang University Zhejiang Provincial Key Lab of Ophthalmology Eye Center of the Second Affiliated Hospital School of Medicine Zhejiang University School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Max-Planck Institute for Polymer Research Ulm University

The fabrication of Gemcitabine(GEM) prodrug was reported to be an effective method to enhance its pancreatic cancer treatment efficiency. Here, a kind of nanocarbon-based materials, nanodiamond(ND), was selected as the nanocarrier of GEM, owing to its outstanding surface properties and non-cytotoxicity. The polyelectrolytes,polyethyleneimine and polyacrylic acid, were used to self-assemble outside ND surface through electrostatic forces, followed by attachment of polyethylene glycol to address better biocompatibility. GEM was conjugated with an enzyme-sensitive peptide gly-phe-leu-gly to build up the controlled release platform. From characterization results of dynamic laser scattering, zeta potential and transmission electron microscope, the significant improvement of ND stability in physiological condition was proved. Non-cytotoxicity of this functionalized ND carriers and cytotoxicity of the prodrug against Bx PC-3 pancreatic cancer cells were indicated by methylthiazolyl tetrazolium(MTT) assay. In vivo experiments also revealed its superior anticancer effect compared with free GEM treatment. Therefore, the combination of polymer coated NDs with high surface capability and enzymeresponsive intracellular GEM release make it possible to realize higher treatment efficiency on pancreatic tumor therapy.

关键词： Nanodiamonds Self-assembly Enzyme-sensitive Gemcitabine prodrug

Traceless photodegradable polymer cocoons for universal protein delivery and light-controlled gene editing

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Science China Chemistry 2024年第2期67卷 664-676页

作者： Huaibin Yu Meron Tsegay Kifle Lili Chen Feihong Xiong Yan Zhang Shangbang Gao Wei Hou Shuliang Chen Weining Zhao yuzhou wu Hubei Engineering Research Center for Biomaterials and Medical Protective Materials Hubei Key Laboratory of Bioinorganic Chemistry&Materia MedicaKey Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan430074China Zhengzhou Research Institute Harbin Institute of TechnologyZhengzhou450000China College of Life Science and Technology Huazhong University of Science and Technology(HUST)Wuhan430074China Institute of Medical Virology School of Basic Medical SciencesWuhan UniversityWuhan430071China College of Pharmacy Shenzhen Technology UniversityShenzhen518118China

Polymer conjugation was found highly valuable in clinic to improve the bioavailability of protein ***,it is still a tremendous challenge to achieve a complete release of original proteins from the conjugated hybrid under external stimulus to recover active proteins in the targeted ***,we report a general light-controlled protein delivery methodology by weaving a photodegradable polymer cocoon around proteins,which could reliably protect them from degradation in the dark while efficiently releasing them under illumination without any residual *** surface charge of the polymer shell is easily tunable to facilitate efficient cell *** versatility of this strategy is demonstrated by the delivery of the Cas9/sg RNA complex that realized light-controlled gene editing both in vitro and in vivo,and such repertoire is of particular value in regard to minimizing the off-target toxicity of CRISPR-Cas9-based gene therapy.

关键词： photodegradable polymer-protein conjugate protein delivery light control gene editing

Programmed albumin nanoparticles regulate immunosuppressive pivot to potentiate checkpoint blockade cancer immunotherapy

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Nano Research 2022年第1期15卷 593-602页

作者： Liandong Feng Li Yang Longjie Li Junying Xiao Nana Bie Chao Xu Jun Zhou Hongmei Liu Lu Gan yuzhou wu Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica Hubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Britton Chance Center for Biomedical Photonics Wuhan National Laboratory for Optoelectronics-Huazhong University of Science and TechnologyWuhan 430074China National Engineering Research Center for Nanomedicine College of Life Science and TechnologyHuazhong University of Science and TechnologyWuhan 430074China

The therapeutic efficacy of programmed cell death protein 1/programmed cell death-ligand 1(PD-1/PD-L1)blockade immunotherapy is extremely dampened by complex immunosuppressive mechanisms including regulatory T cells(Treg),M2 macrophages(M2),and prostaglandin E2(PGE2).The pivotal roles of PGE2 have been recognized by directly inactivating CD8+T cells and indirectly inducing Treg and ***,PGE2 abolishment through inactivating cyclooxygenase-2(COX-2)could be robust to sensitize tumour toward anti-PD-1/PD-L1 immunotherapy,which has gone into clinical ***,exploring this promising strategy in nanomedicine to enhance immunotherapy remains *** key challenge to synergistically combine COX-2 inhibition and anti-PD-1/PD-L1 lies in the different pharmacokinetic profiles and the spatial obstacles since PD-1/PD-L1 interaction occurs extracellularly and COX-2 locates ***,the programmed release nanoparticles(termed as Cele-BMS-NPs)are rationally designed,which are composed of pH-sensitive human serum albumin derivative,BMS-202 compound as PD-1/PD-L1 inhibitor,glutathione(GSH)-activatable prodrug of celecoxib(COX-2 inhibitor).The in vitro experiments demonstrate that this smart Cele-BMS-NPs could extracellularly release BMS-202 under the acidic tumour microenvironment,and the intracellularly release of celecoxib in response to the elevated GSH concentration inside tumour *** systemic administration,the intratumoral infiltration of CD8+T cells is significantly enhanced and meanwhile immunosuppressive M2,Treg,and PGE2 are reduced,thereby eliciting the anti-tumour immune responses toward low immunogenic tumours and postsurgical tumour recurrences.

关键词： dual-responsive nanoparticles programmed release albumin biopolymer immunosuppressive environment immune checkpoint blockade therapy

Directional design and synthesis of high-yield hollow Fe-MFI zeolite encapsulating ultra-small Fe_(2)O_(3) nanoparticles by using mother liquid

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Nano Research 2021年第11期14卷 4304-4313页

作者： Yi Zhai Fumin Wang Xubin Zhang Guojun Lv yuzhou wu Tao Jiang Qing Zhang Mengyue Li Mengyao Li Yongkui Liu School of Chemical Engineering and Technology Tianjin UniversityTianjin300350China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang212003China

How to directionally design the hollow zeolite via a green route is of great significance. Here, we successfully synthesized the hollow Fe-silicate-1 encapsulated ultra-small Fe_(2)O_(3) nanoparticles (2.5 nm) with higher yield (85.2%) by mother liquid than traditional dissolution-recrystallization for the first time, which was achieved by precisely regulating the number and distribution of defects in zeolite and cleverly utilizing the TPAOH and nuclei in mother liquor. The effects of synthetic temperature, synthetic period and addition amount of parent zeolite on the formation of hollow zeolite have been investigated and the effect of synthetic conditions on the defects in parent zeolite has been also firstly quantified. The corresponding formation mechanism has been proposed. The abundant inner defects provided by the zeolite synthesized at 130 °C for 1 day and large amount of TPAOH remaining in mother liquid are conducive to the formation of hollow zeolite. Meanwhile, both parent zeolite and nuclei (4-, 5-member rings and structure units) in mother liquid obtained at 130 °C play the crucial roles in enhancing the zeolite yield. Notably, Fe_(2)O_(3) nanoparticles could decompose into small fragments by the interaction with nuclei in mother liquid. Partial ultra-small Fe_(2)O_(3) nanoparticles would be encapsulated in cavity and the rest could be inserted in the zeolite framework, which is significantly different from the conventional dissolution-recrystallization mechanism. The obtained encapsulated catalyst shows the superior catalytic performance and stability in phenol and tetracycline degradation reactions.

关键词： mother liquid hollow zeolite high yield defect sites degradation reaction

DNA origami-based nano-hunter enriches low-abundance point mutations by targeting wild-type gene segments

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Chinese Chemical Letters 2022年第4期33卷 2052-2056页

作者： Longjie Li Kejun Dong Xinyu Wang Meizhou Zhang Jun Li Andreas KNussler Xianjin Xiao Hongbo Wang yuzhou wu School of Life Science and Technology Wuhan Polytechnic UniversityWuhan 430023China Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica Hubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Department of Obstetrics and Gynecology Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430022China Institute of Reproductive Health Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China Department of Breast Surgery Second Hospital of Jilin UniversityChangchun 130041China Siegfried Weller Institute for Trauma Research Eberhard-Karls-Universitat TubingenSchnarrenbergstr.95D-72076TubingenGermany

Point mutations can be used as biomarkers to perform diagnosis for diseases. In this study, a nanorobot for low-abundance point mutation enrichment was constructed using DNA origami. The novel design achieved limits of detection of 0.1% and 1% for synthesized DNA samples and clinical gene samples, respectively. Resettability was a key property of this method, which also involved a simpler process, lower cost and shorter detection duration than traditional enrichment methods. This novel DNA nanorobot may enable the detection of tumor markers, potentially facilitating early cancer diagnosis.

关键词： Low-abundance point mutation Cancer diagnosis DNA nano-hunter Enrichment Resettability

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基于设计文化视角的晚明陶瓷品鉴研究

装饰 2019年第9期 132-133页

作者：伍玉宙淮阴工学院设计艺术学院

赏鉴与收藏在晚明文人文化中扮演着极为重要的角色,诸如晚明的社会阶层、雅俗分野、审美尺度、生活趣味与身份诉求等均可从中察见端倪。本文以当时的陶瓷品鉴文献为线索,构建"器物特征、评价标准、生活风格、文士身份"相互反映框架,对... 详细信息

赏鉴与收藏在晚明文人文化中扮演着极为重要的角色,诸如晚明的社会阶层、雅俗分野、审美尺度、生活趣味与身份诉求等均可从中察见端倪。本文以当时的陶瓷品鉴文献为线索,构建"器物特征、评价标准、生活风格、文士身份"相互反映框架,对四者共同构成的整体性形象进行呈现,以揭示陶瓷品鉴过程中的特定社会关系,进而探讨基于陶瓷鉴赏而形成的设计文化研究框架在当前消费语境下进行拓展的价值。

关键词：晚明陶瓷品鉴雅俗文人消费

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产品开发设计课程中的情境体验导入

装饰 2016年第11期 138-139页

作者：伍玉宙淮阴工学院设计学院

在体验经济背景下,情感体验已经成为设计中的重要因素。笔者以淮阴工学院工业设计专业的产品开发设计课程为样本,就课程改革的理念、情境体验导入的方式、课程内容的安排以及学生的学习反馈等方面对为什么及如何在本课程中融入体验因素... 详细信息

在体验经济背景下,情感体验已经成为设计中的重要因素。笔者以淮阴工学院工业设计专业的产品开发设计课程为样本,就课程改革的理念、情境体验导入的方式、课程内容的安排以及学生的学习反馈等方面对为什么及如何在本课程中融入体验因素进行了分析。

关键词：产品开发设计情境体验

Spatiotemporal Control of Protein Labeling in Live Cells Enabled by a Photoreactive Ligand-Directed Probe

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Spatiotemporal Control of Protein Labeling in Live Cells Ena...