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Synthetic fungal melanin UV absorbers

Science China Chemistry 2024年第9期67卷 3098-3110页

作者： Chao Wang Rong Zhang Jianhua Zhang Xueqian Zhang Hengjie Zhang Huan Cao Zhen Yang Yiwen Li College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China Department of Radiology Huaxi MR Research CenterFunctional and Molecular Imaging Key Laboratory of Sichuan ProvinceNational Clinical Research Center for GeriatricsWest China HospitalSichuan UniversityChengdu 610041China

Agents with robust ultraviolet(UV)absorption capabilities play a vital role in safeguarding organisms and inorganic materials from UV ***,the synthetic procedures towards these UV absorbers are usually lengthy and complicated,accompanied by undesirable side reactions and the generation of toxic *** nature,allomelanin,a class of melanins variant found in melanized fungi near the Chernobyl nuclear power plant,plays crucial roles in the cell wall of melanized fungi,offering resistance to harsh external environments and promising UV resistance ***,allomelanin can be rapidly biosynthesized via the polymerization of 1,8-dihydroxynaphthalene in presence of enzymes in *** by this,we report here a green enzymatic polymerization strategy to efficiently and eco-friendly synthesize polydihydroxynaphthalene(PDHN)-based artificial allomelanin nanoparticles(NPs)with interesting *** calculations and experimental results demonstrated that the PDHN NPs exhibited excellent UVabsorption capacity,surpassing another widely used artificial melanin,polydopamine(PDA).Moreover,the light absorption mechanism of PDHN NPs was systematically elucidated for the first ***,the PDHN NPs were incorporated with polyvinyl alcohol(PVA)to create an anti-aging composite film with significantly enhanced UV shielding *** potential of these composite films in safeguarding plants from UV damage was meticulously ***,these PDHN NPs were first found to produce hydroxyl radicals(·OH)under UV irradiation,offering antibacterial properties that expand their potential applications.

关键词： melanin artificial allomelanin nanoparticles green synthesis UV absorption antibacterial

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Structural disruption of melanin-like polymers with boosted UV protection

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Science China Chemistry 2024年第5期67卷 1653-1663页

作者： Zhen Yang Xianheng Wang Wanjie Bai Zikun Zou Haoxing Wu Yiwen Li Department of Radiology Huaxi MR Research CenterFunctional and Molecular Imaging Key Laboratory of Sichuan ProvinceNational Clinical Research Center for GeriatricsWest China HospitalSichuan UniversityChengdu 610041China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China

Manipulating the energy structure of materials represents an efficient way to regulate their light absorption behaviors. For example, constructing donor-acceptor(D-A) structures to increase the polarizability and reduce the energy bandgap of local molecules has been widely used in the field of organic photovoltaics with ordered structures. Remarkably, even in disordered and chaotic systems such as melanin-like polydopamine(PDA), visible and near-infrared light absorption can be significantly improved using this strategy. However, there has been a noticeable dearth of research on the ultraviolet(UV) light absorption regulation of bioinspired polymers with disordered and chaotic architectures by tailoring the D-A microstructures. In this study, a series of benzoheterocyclic molecules with strong electron-donating features screened by molecular simulation calculations were involved in disrupting the D-A structures within PDA. The destruction of D-A structures promoted the increase of the energy band gap and finally boosted the UV absorption of PDA. The resulting PDA nanoparticles with enhanced UV absorption were further employed to fabricate UV shielding composite films to protect the growth of plants from harmful UV radiation. This research may open up new avenues for structural disruption of bioinspired polymers for enhanced photoprotection applications.

关键词： melanin-like polymers polydopamine D-A structure UV absorption photoprotection

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Dendritic nanomedicine enhances chemoimmunotherapy by disturbing metabolism of cancer-associated fibroblasts for deep penetration and activating function of immune cells

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Acta Pharmaceutica Sinica B 2024年第8期14卷 3680-3696页

作者： Yunkun Li Xiaoding Shen Haitao Ding Yuxin Zhang Dayi Pan Liping Su Yahui Wu Zaixiang Fang Jie Zhoua Qiyong Gong Kui Luo Department of Radiology Huaxi MR Research Center(HMRRC)Frontiers Science Center for Disease-Related Molecular NetworkState Key Laboratory of BiotherapyWest China HospitalSichuan UniversityChengdu 610041China Functional and Molecular Imaging Key Laboratory of Sichuan Province and Research Unit of PsychoradiologyChinese Academy of Medical SciencesChengdu 610041China Department of Radiology West China Xiamen Hospital of Sichuan UniversityXiamen 361021China

Inefficient drug penetration hurdled by the stroma in the tumor tissue leads to a diminished therapeutic effect for drugs and a reduced infiltration level of immune ***,we constructed a PEGylated dendritic epirubicin(Epi)prodrug(Epi-P4D)to regulate the metabolism of cancer-associated fibroblasts(CAFs),thus enhancing Epi penetration into both multicellular tumor spheroids(MTSs)and tumor tissues in mouse colon cancer(CT26),mouse breast cancer(4T1)and human breast cancer(MDA-MB-231)*** cytotoxicity against CT26 MTSs and remarkable antitumor efficacy of Epi-P4D were ascribed to reduced fibronectin,α-SMA,and collagen ***,thinning of the tumor tissue stroma and efficient eradication of tumor cells promoted the immunogenic cell death effect for dendritic cell(DC)maturation and subsequent immune activation,including elevating the CD4^(+)T cell population,reducing CD4^(+)and CD8^(+)T cell hyperactivation and exhaustion,and amplifying the natural killer(NK)cell proportion and effectively activating *** a result,this dendritic nanomedicine thinned the stroma of tumor tissues to enhance drug penetration and facilitate immune cell infiltration for elevated antitumor efficacy.

关键词： Dendritic prodrug Enhanced penetration Metabolic intervention Cancer-associated fibroblasts Immunogenic cell death Chemotherapy Immunotherapy Immune microenvironment reconstitution

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N-Heterocyclic carbene-catalyzed enantioselective(dynamic) kinetic resolutions and desymmetrizations

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Science China Chemistry 2024年第2期67卷 482-511页

作者： Yi Zhang Hui Cai Xiuhai Gan Zhichao Jin National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityHuaxi DistrictGuiyang550025China

N-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically *** content is organized according to the activation modes involved i... 详细信息

关键词： N-heterocyclic carbene kinetic resolution dynamic kinetic resolution desymmetrization organocatalysis

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Branched glycopolymer prodrug-derived nanoassembly combined with a STING agonist activates an immuno-supportive status to boost anti-PD-L1 antibody therapy

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2194-2209页

作者： Zhilin Li Qianfeng Zhang Zhiqian Li Long Ren Dayi Pan Qiyong Gong Zhongwei Gu Hao Cai Kui Luo Department of Radiology Huaxi MR Research Center(HMRRC)Clinical Research Center for BreastDepartment of Breast SurgeryDepartment of Thoracic Surgery and Institute of Thoracic OncologyFrontiers Science Center for Disease-Related Molecular NetworkState Key Laboratory of BiotherapyWest China Hospital Sichuan UniversityChengdu 610041China Functional and Molecular Imaging Key Laboratory of Sichuan Province and Research Unit of PsychoradiologyChinese Academy of Medical SciencesChengdu 610041China Department of Radiology West China Xiamen Hospital of Sichuan UniversityXiamen 361021China Key Laboratory of Medicinal Chemistry for Natural Resource Ministry of EducationYunnan Key Laboratory of Research and Development for Natural ProductsSchool of PharmacyYunnan UniversityKunming 650500China

Despite the great potential of anti-PD-L1 antibodies for immunotherapy,their low response rate due to an immunosuppressive tumor microenvironment has hampered their *** address this issue,we constructed a cell membrane-coated nanosystem(mB4S)to reverse an immunosuppressive microenvironment to an immuno-supportive one for strengthening the anti-tumor *** this system,Epirubicin(EPI)as an immunogenic cell death(ICD)inducer was coupled to a branched glycopolymer via hydrazone bonds and diABZI as a stimulator of interferon genes(STING)agonist was encapsulated into *** internalization of mB4S,EPI was acidic-responsively released to induce ICD,which was characterized by an increased level of calreticulin(CRT)exposure and enhanced ATP ***,diABZI effectively activated the STING *** with mB4S in combination with an anti-PD-L1 antibody elicited potent immune responses by increasing the ratio of matured dendritic cells(DCs)and CD8+T cells,promoting cytokines secretion,up-regulating M1-like tumor-associated macrophages(TAMs)and down-regulating immunosuppressive myeloid-derived suppressor cells(MDSCs).Therefore,this nanosystem for co-delivery of an ICD inducer and a STING agonist achieved promotion of DCs maturation and CD8+T cells infiltration,creating an immuno-supportive microenvironment,thus potentiating the therapy effect of the anti-PD-L1 antibody in both 4T1 breast and CT26 colon tumor mice.

关键词： Glycopolymer Polymer prodrug Immunogenic cell death Nanoassembly Epirubicin STING pathway Immuno-supportive microenvironment Immunotherapy

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Hyperpolarized ^(13)C mrI in hepatocellular carcinoma:Unmet questions during clinical translation

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Chinese Medical Journal 2024年第13期137卷 1516-1518页

作者： Zheng Ye Bin Song Christoffer Laustsen Department of Radiology West China HospitalSichuan UniversityChengduSichuan 610041China The mr Research center Department of Clinical MedicineAarhus UniversityAarhus N 8200Denmark

Hyperpolarized(HP)^(13)C magnetic resonance imaging(mrI)is a powerful molecular imaging *** dissolution dynamic nuclear polarization(d-DNP),it can achieve dramatic signal increase and allows for dynamic and quantitative investigation of real-time metabolism in vivo.[1]The typical HP^(13)C mrI workflow begins with formulating the^(13)C probe,and then placing it in the hyperpolarization equipment to achieve the desired signal amplification level,which typically amounts to an increase in the mrI signal by more than 10,000 *** subsequent data acquisition is supported by a specialized^(13)C coil and^(13)C acquisition sequence,and finally quantitative and visualized metabolic information is obtained through a post-processing *** date,research of HP^(13)C mrI has focused on diabetes,cardiovascular diseases,and cancers,[2]showing great promises in tumor detection and the evaluation of therapeutic efficacy.

关键词： metabolism polarized specialized

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A nonenzymatic electrochemical sensor for the detection of hydrogen peroxide in vitro and in vivo fibrosis models

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Chinese Chemical Letters 2024年第3期35卷 394-398页

作者： Hongyao Liu Yan Yu Taixiong Xue Cailing Gan Yuting Xie Doudou Wang Peilin Li Zhiyong Qian Tinghong Ye Department of Gastroenterology and Hepatology Sichuan University-University of Oxford Huaxi Joint Centre for Gastrointestinal Cancer and Frontiers Science Center for Disease-Related Molecular NetworkState Key Laboratory of BiotherapyWest China HospitalSichuan UniversityChengdu 610041China Department of Biotherapy Cancer Center and State Key Laboratory of BiotherapyWest China HospitalSichuan UniversityChengdu 610041China

Fibrosis occurs due to the excessive deposition of extracellular matrix caused by cell *** various types of tissue injury,the dysregulation of the internal response can eventually lead to the destruction of organ structure and *** is increasing evidence that oxidative stress,which is characterized by excessive production of hydrogen peroxide(H_(2)O_(2)),is an important cause of ***,we synthesized a biosensitive and efficient electrochemical H_(2)O_(2)sensor based on PtNi nanoparticle-doped N-reduced graphene oxide(PtNi-N-rGO)to detect H_(2)O_(2)released from transforming growth factorβ1(TGFβ1)-induced *** addition,the sensor could easily detect changes in H_(2)O_(2)in the lung and bronchoalveolar lavage fluid(BALF)of mice with pulmonary ***,the sensor could also detect H_(2)O_(2)in activated hepatic stellate cells and the liver of carbon tetrachloride(CCl_(4))-induced liver ***,the alterations in H_(2)O_(2)detected by the sensor were consistent with nicotinamide adenine dinucleotide phosphate oxidase 4(NOX4)protein expression and the staining results of pathological *** together,these results highlight the use of H_(2)O_(2)sensors for the rapid detection of fibrosis and facilitate the rapid evaluation of antifibrotic drug candidates.

关键词： Fibrosis H_(2)O_(2) Electrochemical sensor NOX4 Nintedanib

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A biocompatible Horner-Wadsworth-Emmons(HWE)reaction triggered by a bioorthogonal proximity-induced platform

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Chinese Chemical Letters 2024年第8期35卷 217-220页

作者： Yayue Wang Haojie Yang Jie Li Qiao Kong Siming Zhou Hongbao Sun Lili Pan Qiyong Gong Ping Feng Haoxing Wu Department of Radiology and huaxi mr Research center(HmrRC) Functional and Molecular Imaging Key Laboratory of Sichuan ProvinceFrontiers Science Center for Disease Related Molecular NetworkWest China HospitalSichuan UniversityChengdu 610041China Key Laboratory of Drug-Targeting and Drug Delivery System of the Education Ministry and Sichuan Province Sichuan UniversityChengdu 610041China Department of Nuclear Medicine Laboratory of Clinical Nuclear MedicineWest China HospitalSichuan UniversityChengdu 610041China Reseacrch Unit of Psychoradiology Chinese Academy of Medical SciencesChengdu 610041China Department of Pharmacy West China HospitalSichuan UniversityChengdu 610041China Clinical Trial center and National Medical Products Administration Key Laboratory for Clinical Research and Evaluation of Innovative Drugs West China HospitalSichuan UniversityChengdu 610041China

Here,we present a novel bioorthogonal platform that enables precise positioning of attached moieties in close proximity,thereby facilitating the discovery and optimization of biocompatible *** this platform,we achieve a Horner-Wadsworth-Emmons(HWE)reaction under physiological conditions,generating a fluorophore in situ with a yield of up to 93%.This proximity platform should facilitate the discovery of various types of biocompatible reactions,making it a versatile tool for biomedical applica-tions.

关键词： Biocompatible reactions Horner-Wadsworth-Emmons reaction Bioorthogonal reactions Tetrazines Proximity effects

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Deep learning model based on PET/CT and combination with Cox proportional hazard model for predicting progression of lung invasive adenocarcinoma after surgery

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中国医学影像技术 2024年第8期40卷 1194-1198页

作者： LI Yingci WU Dongbo GONG Feifei Department of PET/CT-mr center Harbin Medical University Cancer HospitalHarbin 150081China Department of Radiology Harbin Medical University Cancer HospitalHarbin 150081China Department of Radiology Harbin Chest HospitalHarbin 150056China

Objective To observe the efficacy of deep learning(DL)model based on PET/CT and its combination with Cox proportional hazard model for predicting progressive disease(PD)of lung invasive adenocarcinoma within 5 years after *** The clinical,PET/CT and 5-year follow-up data of 250 patients with lung invasive adenocarcinoma were retrospectively *** to PD or not,the patients were divided into the PD group(n=71)and non-PD group(n=179).The basic data and PET/CT findings were compared between groups,among which the quantitative variables being significant different between groups were transformed to categorical variables using receiver operating characteristic(ROC)curve and corresponding cut-off *** Cox proportional hazard model was used to select independent predicting factors of PD of lung invasive adenocarcinoma within 5 years after *** patients were divided into training,validation and test sets at the ratio of 6∶2∶2,and PET/CT data in training set and validation set were used to train model and tuning parameters to build the PET/CT DL model,and the combination model was built in serial connection of DL model and the predictive *** test set,the efficacy of each model for predicting PD of lung invasive adenocarcinoma within 5 years after surgery was assessed and compared using the area under the curve(AUC).Results Patients'gender and smoking status,as well as the long diameter,SUV max and SUV mean of lesions measured on PET images,the long diameter,short diameter and type of lesions showed on CT were statistically different between groups(all P4.15(HR=5.249[1.062,25.945],P=0.042)were both predictors of PD of lung invasive adenocarcinoma within 5 years after *** test set,the AUC of PET/CT DL model for predicting PD was 0.847,of the combination model was 0.890,of the latter was higher than of the former(P=0.036).Conclusion DL model based on PET/CT

关键词： adenocarcinoma of lung positron-emission tomography and computed tomography deep learning disease progression

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Staging liver fibrosis with various diffusion-weighted magnetic resonance imaging models

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World Journal of Gastroenterology 2024年第9期30卷 1164-1176页

作者： Yan-Li Jiang Juan Li Peng-Fei Zhang Feng-Xian Fan Jie Zou Pin Yang Peng-Fei Wang Shao-Yu Wang Jing Zhang Department of Magnetic Resonance Imaging The Second Hospital&Clinical Medical SchoolLanzhou UniversityLanzhou 730030Gansu ProvinceChina Second Clinical School Lanzhou UniversityLanzhou 730030Gansu ProvinceChina Gansu Province Clinical Research center for Functional and Molecular Imaging The Second Hospital&Clinical Medical SchoolLanzhou UniversityLanzhou 730030Gansu ProvinceChina Department of Hepatology The Second Hospital&Clinical Medical SchoolLanzhou UniversityLanzhou 730030Gansu ProvinceChina mr Scientific Marketing Siemens HealthineersXi’an 710065Shaanxi ProvinceChina

BACKGROUND Diffusion-weighted imaging(DWI)has been developed to stage liver ***,its diagnostic performance is inconsistent among ***,it is worth studying the diagnostic value of various diffusion models for liver fibrosis in one *** To evaluate the clinical potential of six diffusion-weighted models in liver fibrosis staging and compare their diagnostic *** This prospective study enrolled 59 patients suspected of liver disease and scheduled for liver biopsy and 17 healthy *** participants underwent multi-b value *** main DWI-derived parameters included Mono-apparent diffusion coefficient(ADC)from mono-exponential DWI,intravoxel incoherent motion model-derived true diffusion coefficient(IVIM-D),diffusion kurtosis imaging-derived apparent diffusivity(DKI-MD),stretched exponential model-derived distributed diffusion coefficient(SEM-DDC),fractional order calculus(FROC)model-derived diffusion coefficient(FROC-D)and FROC model-derived microstructural quantity(FROC-μ),and continuous-time random-walk(CTRW)model-derived anomalous diffusion coefficient(CTRW-D)and CTRW model-derived temporal diffusion heterogeneity index(CTRW-α).The correlations between DWI-derived parameters and fibrosis stages and the parameters’diagnostic efficacy in detecting significant fibrosis(SF)were assessed and *** CTRW-D(r=-0.356),CTRW-α(r=-0.297),DKI-MD(r=-0.297),FROC-D(r=-0.350),FROC-μ(r=-0.321),IVIM-D(r=-0.251),Mono-ADC(r=-0.362),and SEM-DDC(r=-0.263)were significantly correlated with fibrosis *** areas under the ROC curves(AUCs)of the combined index of the six models for distinguishing SF(0.697-0.747)were higher than each of the parameters alone(0.524-0.719).The DWI models’ability to detect SF was *** combined index of CTRW model parameters had the highest AUC(0.747).CONCLUSION The DWI models were similarly valuable in distinguishing SF in patients with liver *** combined index of CTRW paramet

关键词： Liver fibrosis Magnetic resonance imaging Diffusion-weighted magnetic resonance Liver biopsy Significant fibrosis

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