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Multifunctional properties of a polar spin chain compound[N(C_(3)H_(7))_(4)][Cu(C_(8)H_(4)NO_(4))]·H_(2)O exhibiting both one-dimensional magnetism and nonlinear optical activity

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Chinese Chemical Letters 2024年第2期35卷 622-625页

作者： Ang Li Yanhong Wang Haotian Tian Alimujiang Yalikun Yves Journaux Min Luo Hongcheng Lu key laboratory of material chemistry for Energy Conversion and Storage School of Chemistry and Chemical EngineeringHubei Key Laboratory of Bioinorganic Chemistry & Materia MedicaHuazhong University of Science and TechnologyWuhan 430074China key laboratory of optoelectronic materials chemistry and Physics Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 35002China Institut Parisien de Chimie Moléculaire IPCMSorbonne UniversitéCNRSParis F-75252France

Functional materials with multiple properties are urgent to be explored to reach high requirements for applications *** this work,a new multifunctional one-dimensional(1D)chain compound[N(C_(3)H_(7))_(4)][Cu(ohpma)]·H_(2)O 1(ohpma=deprotonated N-(2-hydoxyphenyl)oxamic acid)exhibiting both 1D antiferromagnetic and nonlinear optical properties,which are both originated from the same polar[Cu(C_(8)H_(4)NO_(4))]magnetic units,has been successfully synthesized by evaporation at room ***-polydentate nature of the(ohpma)3−ligand with constrained tridentate and bidentate coordination sites conducts Cu^(2+)ions coordinating in different geometries and forms 1D chains along the c axis,which are further separated by the[N(C_(3)H_(7))_(4)]+*** the 1D magnetic chains further exhibit noncentrosymmetric polar *** optical study shows polar compound 1 exhibits a discernible second-harmonic generation(SHG)efficiency and the calculation of the partial density of states indicates that the SHG efficiency of 1 is mainly originated from the polar[Cu(C_(8)H_(4)NO_(4))]magnetic ***,magnetic susceptibility shows a broad maximum around 70 K with strong intrachain interaction of J/k B=−113.0 K but no long-range order is observed down to 2 K,suggesting that 1 shows a good 1D *** good 1D magnetism and SHG activity suggest that 1 could be as a potential multifunctional material,particularly.

关键词： Multifunctional properties Magnetic property Nonlinear optical property Evaporation One-dimensional chain

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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

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Alectinib: a novel second generation anaplastic lymphoma kinase(ALK) inhibitor for overcoming clinically-acquired resistance

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Acta Pharmaceutica Sinica B 2015年第1期5卷 34-37页

作者： Zilan Song Meining Wang Ao Zhang CAS key laboratory of Receptor Research Synthetic Organic & Medicinal Chemistry LaboratoryShanghai Institute of Materia Medica (SIMM) Chinese Academy of Sciences

The development of inhibitors for the tyrosine anaplastic lymphoma kinase (ALK) has advanced rapidly, driven by biology and medicinal chemistry. The first generation ALK inhibitor crizotinib was granted US FDA approval with only four years of preclinical and clinical testing. Although this drug offers significant clinical benefit to the ALK-positive patients, resistance has been developed through a variety of mechanisms. In addition to ceritinib, alectinib is another second-generation ALK inhibitor launched in 2014 in Japan. This drug has a unique chemical structure bearing a 5H-benzo[b] carbazol-11(611)-one structural scaffold with an IC50 value of 1.9 nmol/L, and is highly potent against ALK bearing the gatekeeper mutation L1196M with an IC50 of 1.56 nmoL/L. In the clinic, alectinib is highly efficacious in treatment of ALK-positive non-small cell lung cancer (NSCLC), and retains potency to combat crizotinib-resistant ALK mutations L11.96.M, F1174L, R1275Q and C1156Y. (C) 2015 Chinese Pharmaceutical Association and Institute of materia medica, Chinese Academy of medical Sciences. Production and hosting by Elsevier B.V. All rights reserved.

关键词： Tyrosine anaplastic lymphoma kinase Alectinib Crizotinib Non-suaall cell lung cancer Resistance ALK mutations EML4-ALK

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Targeting sphingosine-1-phosphate signaling for cancer therapy

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Science China(Life Sciences) 2017年第6期60卷 585-600页

作者： Zuoquan Xie Hong Liu Meiyu Geng Division of Antitumor Pharmacology State Key Laboratory of Drug ResearchShanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China Division of chemistry State Key Laboratory of Drug ResearchShanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China

Sphingosine-1-phosphate(S1P) is a potent pleotropic bioactive lipid mediator involved in immune cell trafficking, cell survival,cell proliferation, cell migration, angiogenesis and many other cellular processes. S1 P either activates S1 P receptors(S1PR1-5) through "inside-out signaling" or acts directly on intracellular targets to regulate various cellular processes. In the past two decades, much progress has been made in exploring S1 P signaling and its pathogenic roles in diseases as well as in developing modulators of S1 P signaling, including S1 P agonists, S1 P antagonists and sphingosine kinase(SphK) *** and S1 P have been defined as reciprocal regulators of cell fate, and S1 P signaling has been shown to be crucial for the pathogenesis of various diseases, including autoimmune diseases, inflammation and cancer; therefore, targeting S1 P signaling may curtail the process of pathogenesis and serve as a potential therapeutic target for the treatment of these diseases. In this review, we describe recent advances in our understanding of S1 P signaling in cancer development(particularly in inflammationassociated cancer) as well as in innate and adaptive immunity, and we also discuss modulators of S1 P signaling in cancer treatment.

关键词： sphingosine-1-phosphate sphingosine ceramide cancer inflammation immunity

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One-dimensional and two-dimensional nanomaterials for the detection of multiple biomolecules

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Chinese Chemical Letters 2019年第9期30卷 1557-1564页

作者： Quan Wang Xudong Wang Min Xu Xiaoding Lou Fan Xia Engineering Research Center of Nano-Geomaterials of Ministry of Education Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430074 China hubei key laboratory of bioinorganic chemistry & materia medica School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China Zhejiang Institute China University of Geosciences Wuhan Hangzhou 311305 China

The complexity of biological samples determines that the detection of a single biomolecule is unable to satisfy actual needs. Moreover, the "false positives" results caused by a single biomolecule detections easily leads to erroneous clinical diagnosis and treatment. Thus, it is important for the homogenous quantification of multiple biomolecules in not only basic research but also practical application. As a consequent, a large number of literatures have been exploited to monitor multiple biomolecules in homogenous solution, enabling facilitating the development of the disease diagnosis, treatment as well as drug discovery. One-dimensional nanomaterials and two-dimensional nanomaterials have special physical and chemical properties, such as good electrochemical properties, stable structure, large specific surface area, and biocompatibility, which are widely used in electrochemical and fluorescent detection of biomolecules. This tutorial review highlights the recent development for the detection of multiple biomolecules by using nanomaterials including one-dimensional materials(1DMs) as well as twodimensional materials(2DMs).

关键词： One-dimensional nanomaterials Two-dimensional nanomaterials Detection Multiple targets Biomolecules

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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

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Applying high-performance computing in drug discovery and molecular simulation

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National Science Review 2016年第1期3卷 49-63页

作者： Tingting Liu Dong Lu Hao Zhang Mingyue Zheng Huaiyu Yang Yechun Xu Cheng Luo Weiliang Zhu Kunqian Yu Hualiang Jiang State key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of Sciences

In recent decades, high-performance computing(HPC) technologies and supercomputers in China have significantly advanced, resulting in remarkable achievements. Computational drug discovery and design,which is based on HPC and combines pharmaceutical chemistry and computational biology, has become a critical approach in drug research and development and is financially supported by the Chinese government. This approach has yielded a series of new algorithms in drug design, as well as new software and databases. This review mainly focuses on the application of HPC to the fields of drug discovery and molecular simulation at the Chinese Academy of Sciences, including virtual drug screening, molecular dynamics simulation, and protein folding. In addition, the potential future application of HPC in precision medicine is briefly discussed.

关键词： high-performance computing computational drug discovery and design virtual screening molecular dynamics simulation protein folding

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A Conductive Dinuclear Cuprous Complex Mimicking the Active Edge Site of the Copper(100)/(111)Plane for Selective Electroreduction of CO_(2) to C_(2)H_(4) at Industrial Current Density

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Research 2023年第2期2022卷 343-349页

作者： Jin-Meng Heng Hao-Lin Zhu Zhen-Hua Zhao Da-Shuai Huang Jun-Yi Li Pei-Qin Liao Xiao-Ming Chen MOE key laboratory of bioinorganic and Synthetic chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

Inorganic solids are a kind of important catalysts,and their activities usually come from sparse active sites,which are structurally different from inactive ***,the rational optimization of activity depends on studying these active *** is a widely used catalyst and is expected to be a promising catalyst for the electroreduction of CO_(2) to C_(2)H_(4).

关键词： Copper catalyst rational

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Tumor-repopulating cell-derived microparticles elicit cascade amplification of chemotherapy-induced antitumor immunity to boost anti-PD-1 therapy

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Signal Transduction and Targeted Therapy 2023年第11期8卷 5539-5555页

作者： Nana Bie Tuying Yong Zhaohan Wei Qingle Liang Xiaoqiong Zhang Shiyu Li Xin Li Jianye Li Lu Gan Xiangliang Yang National Engineering Research Center for Nanomedicine College of Life Science and TechnologyHuazhong University of Science and Technology430074WuhanChina key laboratory of Molecular Biophysics of the Ministry of Education College of Life Science and TechnologyHuazhong University of Science and Technology430074WuhanChina hubei key laboratory of bioinorganic chemistry and materia medica Huazhong University of Science and Technology430074WuhanChina

Immune checkpoint blockade(ICB)therapy,particularly antibodies targeting the programmed death receptor 1(PD-1)and its ligand(PD-L1),has revolutionized cancer ***,its efficacy as a standalone therapy remains *** ICB therapy in combination with chemotherapy shows promising therapeutic responses,the challenge lies in amplifying chemotherapy-induced antitumor immunity *** relies on efficient drug delivery to tumor cells and robust antigen presentation by dendritic cells(DCs).Here,we developed tumor-repopulating cell(TRC)-derived microparticles with exceptional tumor targeting to deliver doxorubicin(DOX@3D-MPs)for improve anti-PD-1 ***@3D-MPs effectively elicit immunogenic tumor cell death to release sufficient tumor *** shock protein 70(HSP70)overexpressed in DOX@3D-MPs contributes to capturing tumor antigens,promoting their phagocytosis by DCs,and facilitating DCs maturation,leading to the activation of CD8+T ***@3D-MPs significantly enhance the curative response of anti-PD-1 treatment in large subcutaneous H22 hepatoma,orthotopic 4T1 breast tumor and Panc02 pancreatic tumor *** results demonstrate that DOX@3D-MPs hold promise as agents to improve the response rate to ICB therapy and generate long-lasting immune memory to prevent tumor relapse.

关键词： immunity chemotherapy boost

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(5R)-5-hydroxytriptolide inhibits IFN-γ-related signaling

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Acta Pharmacologica Sinica 2006年第12期27卷 1616-1621页

作者： Ru ZHOU~2 Jun-xia WANG~2 Wei TANG~2 Pei-lan HE~2 Yi-fu YANG~2 Yuan-chao LI~3 Xiao-yu LI~2 Jian-ping ZUO~(2,4)2 laboratory of Immunopharmacology and 3 laboratory of chemistry,State key laboratory of Drug Research,Shanghai Institute of materia medica,Shanghai Institutes for Biological Sciences,Chinese Academy of Sciences,Shanghai 201203,China laboratory of Immunopharmacology State Key Laboratory of Drug Research Shanghai Institute of Materia Medica Shanghai Institutes for Biological Sciences Chinese Academy of Sciences Shanghai China laboratory of chemistry State Key Laboratory of Drug Research Shanghai Institute of Materia Medica Shanghai Institutes for Biological Sciences Chinese Academy of Sciences Shanghai China

Aim:(5R)-5-hydroxytriptolide(LLDT-8)displayed anti-arthritis and anti-allogenictransplantation rejection activities in our previous ***,we aim to furtherclarify the effect of LLDT-8 on the pro-inflammatory cytokine IFN-γ.Methods:Tcells were activated with anti-CD3 antibody or concanavalin A(ConA).The ex-pression of cell surface molecules was detected with flow *** werelabeled with carboxyfluorescein diacetate succinimidyl ester(CFSE)to test ***-γ production was determined by enzyme-linked *** proliferation was evaluated by[~3H]-thymidine *** wereimmunized with ovalbumin to assess the in vivo immune ***-PCR andReal-time PCR were applied to determine the mRNA *** protein phos-phorylation levels were detected by Western immunoblot ***:LLDT-8 at 100 nmol/L did not change the CD25,CD69,and CD154 expressions in anti-CD3-stimulated T ***-8 markedly blocked the cell division of CD4 andCD8 T cells after ConA ***-8 inhibited T cell-derived IFN-γ***,LLDT-8 suppressed the ovalbumin-specific T cell prolif-eration and IFN-γ *** anti-CD3-activated T cells,LLDT-8 abrogated themRNA expression of signal transducer and activator of transcriptionl(STAT1),T-box transcription factor,IL-12 receptor β2,STAT4,and interferon regulatory fac-tor 1 in the IFN-γ expression *** blot analysis showed that LLDT-8 blocked the phosphorylation levels of extracellular signal-regulated kinase,stress-activated protein kinase(SAPK)/c-Jun N-terminal kinase,and p38 mitogen-activated protein kinase in anti-CD3 plus anti-CD28-activated T *** addition,LLDT-8 reduced the transcripts of macrophage inflammatory protein(Mip)-1α,Mip-1β,regulated upon activation normally T-cell expressed and secreted,induc-ible protein-10,IFN-inducible T cell a chemoattractant,and monokine induced byIFN-7 in IFN-γ-stimulated murine macrophage cell line Raw 264.7 ***:LLD

关键词： (5R)-5-hydroxytriptolide IFN-γ MAPK chemokine

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