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Science China Chemistry 2024年第9期67卷 3012-3018页

作者： Jia Nie Huanfeng Jiang Chuanle Zhu School of Chemistry and Chemical Engineering Key Lab of Functional Molecular Engineering of Guangdong Province South China University of Technology Guangdong Provincial Key Laboratory of Technique and Equipment for Macromolecular advanced Manufacturing South China University of Technology

The chemoselective epoxidation of electron-deficient olefins in the presence of electron-rich alkene moieties is reported. This chemoselective epoxidation strategy undergoes a conjugated olefin epoxidation and BHT hydroxylation process to give various useful oxiranes in high yields, especially for the 2-substituted 2-trifluoromethyloxiranes. Importantly, this protocol features mild conditions, is transition-metal free, operationally simple, and gram-scalable, and tolerates diverse functional groups. drug candidate HSD-16 is synthesized smoothly by this protocol. Mechanism studies indicate molecular oxygen is the terminal oxidant and the O-source of the oxiranes.

关键词： chemoselective epoxidation alkene fluorine molecular oxygen

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Polyoxometalates based nanocomposites for bioapplications

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Rare Metals 2023年第11期42卷 3570-3600页

作者： Yao Cheng Ke-Jie Qin De-Jin Zang School of Pharmacy and Pharmaceutical Sciences&Institute of Materia Medica National Key Laboratory of Advanced Drug Delivery and SystemShandong First Medical University&Shandong Academy of Medical SciencesNHC Key Laboratory of Biotechnology Drugs(Shandong Academy of Medical Sciences)Key Lab for Rare&Uncommon Diseases of Shandong ProvinceJinan250117China

Health care and medical care have always been dominant topics in human *** field of precision medicine,iatrotechnics revolution and timely on-demand detection have continued to evolve in response to increasing demands from the ***,the emergence of innovative materials and their applications offer promising prospects for advancing global ***(POMs)are negatively-charged molecular metal oxides with well-defined structures,beautiful geometries and nanoscale *** to their vast diversity in composition,structure,nuclearity and charge,they constitute a significant subcategory of inorganic clusters that contain bridging oxygen atoms between two or more metal ***,POMs based nanocomposites have been widely applied in the field of disease diagnosis,anticancer therapy and antibacterial therapy as new generation bioactive *** this review,the recent advances of POMs based nanocomposites in bioapplications are summarized and the future perspectives are discussed.

关键词： Polyoxometalates(POMs) Disease diagnosis Anticancer therapy Antibacterial therapy Biological imaging

Selective nickel-electrocatalyzed benzylic C-H oxygenation of functionalized alkyl arenes

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Chinese Chemical Letters 2024年第2期35卷 396-401页

作者： Shunyao Tang Siyi Wang Dongmei Zhang Xinxing Zhang Guang Yang Yanwei Wang Youai Qiu State Key Laboratory of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin 300071China College of Chemistry Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (RECAST)Frontiers Science Center for New Organic MatterNankai UniversityTianjin 300071China

Herein, a site-selective paired electrochemical C–H oxidation of functionalized alkyl arenes promoted by nickel catalyst is disclosed. A Ni(Ⅱ)-dioxygen species formed in situ efficiently enable the oxidation process under mild conditions with a broad substrate scope with excellent functional group compatibilities,such as free carboxylic acid, aldehyde, halogen(including aryl iodide), amide and amino acid. The use of the nickel catalyst in combination with water provides a safe, green and economical method for oxidation of a range of molecules varying in complexity and drug derivatives, demonstrating its potential application in organic synthesis and the pharmaceutical industry. Reaction outcomes and mechanistic studies revealed the key role of the in situ Ni(Ⅱ)-dioxygen species for the subsequent oxidation of C(sp^(3))–H bonds,and short-lived reactive intermediates(aryl radical cation) was rapidly captured by the combination of a bipolar ultramicroelectrode(BUME) with nano-electrospray ionization mass spectrometry.

关键词： Electrochemical C-H oxidation Functionalized alkyl arenes Paired nickel-electrocatalysis H_(2)O oxidation Ketones

Recent advances in developing active targeting and multi-functional drug delivery systems via bioorthogonal chemistry

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Signal Transduction and Targeted Therapy 2023年第1期8卷 13-37页

作者： Wenzhe Yi Ping Xiao Xiaochen Liu Zitong Zhao Xiangshi Sun Jue Wang Lei Zhou Guanru Wang Haiqiang Cao Dangge Wang Yaping Li State Key Laboratory of drug Research&Center of Pharmaceutics Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China Yantai Key Laboratory of Nanomedicine&advanced Preparations Yantai Institute of Materia MedicaYantai 264000China Shandong Laboratory of Yantai drug Discovery Bohai Rim Advanced Research Institute for Drug DiscoveryYantai 264000China

Bioorthogonal chemistry reactions occur in physiological conditions without interfering with normal physiological *** metabolic engineering,bioorthogonal groups can be tagged onto cell membranes,which selectively attach to cargos with paired groups via bioorthogonal *** to its simplicity,high efficiency,and specificity,bioorthogonal chemistry has demonstrated great application potential in drug *** the one hand,bioorthogonal reactions improve therapeutic agent delivery to target sites,overcoming off-target *** the other hand,nanoparticles and biomolecules can be linked to cell membranes by bioorthogonal reactions,providing approaches to developing multi-functional drug delivery systems(DDSs).In this review,we first describe the principle of labeling cells or pathogenic microorganisms with bioorthogonal *** then highlight recent breakthroughs in developing active targeting DDSs to tumors,immune systems,or bacteria by bioorthogonal chemistry,as well as applications of bioorthogonal chemistry in developing functional bio-inspired DDSs(biomimetic DDSs,cell-based DDSs,bacteria-based and phage-based DDSs)and ***,we discuss the difficulties and prospective direction of bioorthogonal chemistry in drug *** expect this review will help us understand the latest advances in the development of active targeting and multi-functional DDSs using bioorthogonal chemistry and inspire innovative applications of bioorthogonal chemistry in developing smart DDSs for disease treatment.

关键词： functional orthogonal breakthrough

The state-of-the-art of atmospheric pressure plasma for transdermal drug delivery

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Plasma Science and Technology 2024年第4期26卷 9-26页

作者：聂兰兰刘大伟程鹤赵峰卢新培 State key laboratory of advanced electromagnetic engineering and technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074People’s Republic of China School of Chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094People’s Republic of China Department of Thoracic Surgery Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430022People’s Republic of China

Plasma-enhanced transdermal drug delivery(TDD) presents advantages over traditional methods,including painless application, minimal skin damage, and rapid recovery of permeability. To harness its clinical potential, factors related to plasma’s unique properties, such as reactive species and electric fields, must be carefully *** review provides a concise summary of conventional TDD methods and subsequently offers a comprehensive examination of the current state-of-the-art in plasma-enhanced TDD. This includes an analysis of the impact of plasma on HaCaT human keratinocyte cells, ex vivo/in vivo studies, and clinical research on plasma-assisted TDD. Moreover, the review explores the effects of plasma on skin physical characteristics such as microhole formation, transepidermal water loss(TEWL), molecular structure of the stratum corneum(SC), and skin resistance. Additionally, it discusses the involvement of various reactive agents in plasma-enhanced TDD, encompassing electric fields,charged particles, UV/VUV radiation, heat, and reactive species. Lastly, the review briefly addresses the temporal behavior of the skin after plasma treatment, safety considerations, and potential risks associated with plasma-enhanced TDD.

关键词： plasma transdermal drug delivery skin physical characteristics reactive agents

CD47KO/CRT dual-bioengineered cell membrane-coated nanovaccine combined with anti-PD-L1 antibody for boosting tumor immunotherapy

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Bioactive Materials 2023年第4期22卷 211-224页

作者： Shengyang Liu Jiayan Wu Yuanji Feng Xiaoya Guo Tong Li Meng Meng Jie Chen Daquan Chen Huayu Tian School of Pharmacy Key Laboratory of Molecular Pharmacology and Drug Evaluation(Yantai University)Ministry of EducationCollaborative Innovation Center of Advanced Drug Delivery System and Biotech Drugs in Universities of ShandongYantai UniversityYantai264005PR China Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022PR China College of Chemistry and Chemical Engineering Xiamen UniversityXiamen361005PR China

Tumor vaccines trigger tumor-specific immune responses to prevent or treat tumors by activating the hosts’immune systems,and therefore,these vaccines have potential clinical ***,the low immunogenicity of the tumor antigen itself and the low efficiency of the vaccine delivery system hinder the efficacy of tumor vaccines that cannot produce high-efficiency and long-lasting antitumor immune ***,we constructed a nanovaccine by integrating CD47KO/CRT dual-bioengineered B16F10 cancer cell membranes and the unmethylated cytosine-phosphate-guanine(CpG)*** PEI25k was used to load unmethylated cytosine-phosphate-guanine(CpG)through electrostatic adsorption to prepare PEI25k/CpG nanoparticles(PEI25k/CpG-NPs).CD47KO/CRT dual-bioengineered cells were obtained by CRISPR-Cas9 gene editing technology,followed by the cell surface translocation of calreticulin(CRT)to induce immunogenic cell death(ICD)in ***,the extracted cell membranes were coextruded with PEI25k/CpG-NPs to construct the CD47KO/CRT dual-bioengineered cancer cell membrane-coated nanoparticles(DBE@CCNPs).DBE@CCNPs could promote endocytosis of antigens and adjuvants in murine bone marrow derived dendritic cells(BMDCs)and induce their maturation and antigen *** avoid immune checkpoint molecule-induced T cell dysfunction,the immune checkpoint inhibitor,the anti-PD-L1 antibody,was introduced to boost tumor immunotherapy through a combination with the DBE@CCNPs *** combination therapy strategy can significantly alleviate tumor growth and may open up a potential strategy for clinical tumor immunotherapy.

关键词： CRISPR-Cas9 Dual-bioengineered cell membrane Immune checkpoint blockade Nanovaccine Tumor immunotherapy

LADA strategy for the synthesis of unnatural amino acids and direct modifications of peptides

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Science China Chemistry 2023年第6期66卷 1788-1794页

作者： Jun-Liang Zhou Yun-Qi Liu Zhan-Kui Sun Shanghai Frontiers Science Center for drug Target Identification and drug delivery School of Pharmaceutical SciencesShanghai Jiao Tong UniversityShanghai 200240China Shanghai Key Laboratory for Molecular Engineering of Chiral drugs Pharm-X CenterSchool of Pharmaceutical SciencesShanghai Jiao Tong UniversityShanghai 200240China AI Pharma Center Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai 200240China Shanghai Artificial Intelligence Laboratory Shanghai 200232China

Unnatural amino acids(UAAs)are important building blocks in organic synthesis and drug *** are also frequently integrated into peptides or proteins for biological ***,the direct and simplified synthesis of UAAs remains a great *** the same time,vast known peptide modifications are based on carbon-heteroatom *** are no general methods for peptide modifications via the construction of C–C *** address this challenge,herein we propose the LADA strategy,which is composed of two steps:the selective labeling and activation of cysteine residues,the desulfurization to generate carbon-centered radical and the radical addition to alkenes to build C–C *** one-pot protocol has obvious advantages such as good functional group tolerance,biocompatible reaction conditions,and retained *** strategy was successfully utilized for the synthesis of unnatural amino acids and direct modifications of peptides.

关键词： unnatural amino acids peptide modifications desulfurization cysteine radical addition

A pH-responsive nanoparticle delivery system containing dihydralazine and doxorubicin-based prodrug for enhancing antitumor efficacy

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Aggregate 2024年第1期5卷 436-450页

作者： Lianxue Zhang Jianxiang Huang Damiano Buratto Panli Han Zaixing Yang Ruhong Zhou Institute of Quantitative Biology Shanghai Institute for Advanced StudyCollege of Life SciencesZhejiang UniversityHangzhouChina State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)Soochow UniversitySuzhouChina Cancer Center Zhejiang UniversityHangzhouChina Department of Chemistry Columbia UniversityNew YorkNew YorkUSA

The efficacy of nanoparticle(NP)-based drug delivery technology is hampered by aberrant tumor stromal microenvironments(TSMs)that hinder NP ***,the promotion of NP permeation into deep tumor sites via the regulation of tumor microenvironments is of critical ***,we propose a potential solution using a dihydralazine(HDZ)-loaded nanoparticle drug delivery system containing a pH-responsive,cyclic RGD peptide-modified prodrug based on doxorubicin(cRGD-Dex-DOX).With a combined experimental and theoretical approach,we find that the designed NP system can recognize the acid tumor environments and precisely release the encapsulated HDZ into tumor *** can notably downregulate the expression levels of hypoxia-inducible factor 1α(HIF1α),α-smooth muscle actin,and fibronectin through the dilation of tumor blood *** changes in the TSMs enhance the enrichment and penetration of NPs and also unexpectedly promote the infiltration of activated T cells into tumors,suggesting that such a system may offer an effective“multifunctional therapy”through both improving the chemotherapeutic effect and enhancing the immune response to *** vivo experiments on 4T1 breast cancer bearing mice indeed validate that this therapy has the most outstanding antitumor effects over all the other tested control regimens,with the lowest side effects as well.

关键词： antitumor dihydralazine drug delivery system tumor stromal microenvironment vasculature

Electroluminodynamic therapy for the treatment of drug-resistant pathogen infection

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Biomedical Engineering Communications 2024年第1期3卷 21-22页

作者： Si-Wen Du Jin-Gai Jiang Bo-Han Li Hui-Juan Cheng Yan-Ni Song Fang-Fang Wang Dong-Liang Yang Key Laboratory of Flexible Electronics and Institute of advanced Materials School of Physical and Mathematical SciencesNanjing Tech UniversityNanjing 211816China

The administration of antibiotics has been the primary strategy for combating bacterial infections[1,2].However,the widespread and excessive use of antibiotics has resulted in the alarming rise of bacterial resistance,posing a significant threat to human health[3–5].Therefore,it is imperative to exploit innovative treatment strategy.

关键词： treatment infection dynamic

Unveiling new anti-inflammatory mechanisms of nanomaterials

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National Science Review 2023年第12期10卷 40-42页

作者： Zhen Gu Liangzhu Laboratory College of Pharmaceutical Sciences National Key Laboratory of Advanced Drug Delivery and Release Systems Zhejiang University MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Jinhua Institute of Zhejiang University Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University

Inflammasome activation is instrumental in clearance of pathogens and damaged cells, playing a pivotal role in maintaining host homeostasis. Nonetheless, it is important to note that inflammasome activation can also be a primary driving factor in autoimmune disease and metabolic dysregulation, encompassing conditions such as Alzheimer’s disease, colitis, type 2 diabetes, gout, and atherosclerosis [1].

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