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Molecule configurations modulate packing array and charge transfer in cocrystal engineering

science China Chemistry 2024年第2期67卷 512-516页

作者： Shenglong An Mengyuan Qiao Xin Jin Xuanying Chen Jianhua Su Lifang Guo Zhiyun Zhang Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CentreFrontiers Science Center for Materiobiology and Dynamic ChemistryEast China University of Science&TechnologyShanghai200237China

Organic cocrystal as an emerging assembly strategy has received increasing attention in constructing multiple functional materials,through continually screening suitable constituent monomers or changing their stoichiometry ratios.However,the role of molecule configuration in the cocrystal field is rarely explored despite the fascinating potential in regulating the packing mode.In this study,the N,N′-diphenyl-5,10-dihydrophenazine derivatives(DPPs) with the flexible scaffold and different methyl substitutions are selected as the donors bearing various molecular configurations.In a simple collaborative way,a series of cocrystals based on DPPs and OFN(octafluoronaphthalene) are fabricated,exhibiting two self-adaptive molecular stacking arrays.X-ray crystallographic analysis and theoretical calculation unveil their different π···π interactions and charge transfer characters,leading to the significant emission redshift up to 125 nm compared with individual DPPs.As a result,controllable molecule stacking structure,tunable emission,and charge transfer properties can be achieved.The study provides a new perspective to reveal the structure-property relationships at the molecular level by controlling the molecule configuration in cocrystal engineering,contributing to the development of cocrystal theoretical physics and organic functional materials.

关键词： cocrystals molecular configuration self-adaptive packing mode charge transfer

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MH-STRALP:A scoring system for prognostication in patients with upper gastrointestinal bleeding

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World Journal of Gastrointestinal Surgery 2024年第3期16卷 790-806页

作者： Jun-Nan Hu Fei Xu Ya-Rong Hao Chun-Yan Sun Kai-Ming Wu Yong Lin Lan Zhong Xin Zeng Department of Gastroenterology Shanghai East HospitalTongji University School of MedicineShanghai 200120China Department of Gastroenterology Shanghai Changzheng HospitalNavy Military Medical UniversityShanghai 200003China

BACKGROUND Upper gastrointestinal bleeding(UGIB)is a common medical emergency and early assessment of its outcomes is vital for treatment decisions.AIM To develop a new scoring system to predict its prognosis.METHODS In this retrospective study,692 patients with UGIB were enrolled from two cen-ters and divided into a training(n=591)and a validation cohort(n=101).The clinical data were collected to develop new prognostic prediction models.The en-dpoint was compound outcome defined as(1)demand for emergency surgery or vascular intervention,(2)being transferred to the intensive care unit,or(3)death during hos-pitalization.The models’predictive ability was compared with previously esta-blished scores by receiver operating characteristic(ROC)curves.RESULTS Totally 22.2%(131/591)patients in the training cohort and 22.8%(23/101)in the validation cohort presented poor outcomes.Based on the stepwise-forward Lo-gistic regression analysis,eight predictors were integrated to determine a new post-endoscopic prognostic scoring system(MH-STRALP);a nomogram was de-termined to present the model.Compared with the previous scores(GBS,Rock-all,ABC,AIMS65,and PNED score),MH-STRALP showed the best prognostic prediction ability with area under the ROC curves(AUROCs)of 0.899 and 0.826 in the training and validation cohorts,respectively.According to the calibration cur-ve,decision curve analysis,and internal cross-validation,the nomogram showed good calibration ability and net clinical benefit in both cohorts.After removing the endoscopic indicators,the pre-endoscopic model(pre-MH-STRALP score)was conducted.Similarly,the pre-MHSTRALP score showed better predictive value(AUROCs of 0.868 and 0.767 in the training and validation cohorts,respectively)than the other pre-endoscopic scores.CONCLUSION The MH-STRALP score and pre-MH-STRALP score are simple,convenient,and accurate tools for prognosis prediction of UGIB,and may be applied for early decision on its management strategies.

关键词： Upper gastrointestinal bleeding Prognosis prediction Retrospective study Nomogram Post-endoscopic model Pre-endoscopic model

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Process analytical technologies and self-optimization algorithms in automated pharmaceutical continuous manufacturing

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Chinese Chemical Letters 2024年第3期35卷 87-95页

作者： Peiwen Liu Hui Jin Yan Chen Derong Wang Haohui Yan Mingzhao Wu Fang Zhao Weiping Zhu State Key Laboratory of Bioreactor Engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Engineering Research Center of Pharmaceutical Process Chemistry Ministry of EducationSchool of PharmacyEast China University of Science and TechnologyShanghai 200237China

The pharmaceutical industry is now paying increased attention to continuous manufacturing.While the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world,the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified personnels.In this review,emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing,i.e.,process analytical technology(PAT)and self-optimizing algorithm.Research work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced,which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.

关键词： Pharmaceutical continuous manufacturing Automation Process analytical technology Self-optimization algorithm

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Engineered plant extracellular vesicles for autoimmune diseases therapy

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Nano Research 2024年第4期17卷 2857-2873页

作者： Ruina Han Yan Wu Yafei Han Xiangfei Liu Han Liu Jiacan Su Institute of Translational Medicine Shanghai UniversityShanghai 200444China Organoid Research Center Shanghai UniversityShanghai 200444China National Center for Translational Medicine(shanghai)SHU Branch Shanghai UniversityShanghai 200444China Department of Orthopedics Shanghai Zhongye HospitalShanghai 200941China Department of Orthopedics Xinhua HospitalShanghai Jiao Tong University School of MedicineShanghai 200092China

Autoimmune diseases(AID)encompass a diverse array of conditions characterized by immune system dysregulation,resulting in aberrant responses of B cells and T cells against the body’s own healthy tissues.Plant extracellular vesicles(PEVs)are nanoscale particles enclosed by phospholipid bilayers,secreted by plant cells,which facilitate intercellular communication by transporting various bioactive molecules.Due to their nanoscale structure,safety,abundant sources,low immunogenicity,high yield,biocompatibility,and effective targeting of the colon and liver,PEVs are regarded as a promising platform for the treatment of AID.This review provides a comprehensive summary of PEV biogenesis,physicochemical and biological properties,internalization mechanisms,isolation methods,and their applications in various diseases,with a specific focus on their potential roles in AID.Additionally,we propose engineering approaches and administration methods for PEVs.Finally,we present an overview of the advantages and challenges associated with utilizing PEVs for the treatment of AID.By gaining a comprehensive understanding of PEVs,we anticipate the development of innovative therapeutic strategies for AID.Natural and engineered PEVs hold substantial promise as a valuable resource for innovative technologies in AID treatment.

关键词： autoimmune diseases plant extracellular vesicles extracellular vesicles engineering modification

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Carbon Dots as“On–Off–On”Fluorescence Sensors for Selective and Consecutive Detection of 4-Nitrophenol and Cerium(IV)in Water Samples

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Journal of Analysis and Testing 2024年第2期8卷 201-209页

作者： Jing Yang Hao Liu Yan Huang Li Li Huajie Liu Yaping Ding Department of Chemistry College of SciencesShanghai UniversityShanghai200444China School of Chemical science and Engineering Tongji UniversityShanghai200092China

An“on–off–on”fluorescence sensor was designed for rapidly and consecutively detecting 4-nitrophenol and cerium(IV)without the use of any labeling materials.The yellow carbon dots were synthesized by a simple one-step hydrothermal approach,and various techniques were applied to investigate the morphology,structure,and optical properties of the carbon dots.Under the optimal experimental conditions,4-nitrophenol rapidly quenched the fluorescence of carbon dots as a result of the inner filter eff ect(IFE).The fluorescence intensity of carbon dots was linear with the concentration of 4-nitrophenol(1–150μmol/L)and the limit of detection was 0.32μmol/L.The fluorescence was gradually recovered as the cerium(IV)concentration(0.5–100μmol/L)increased in CDs/4-NP,and the limit of detection was 0.16μmol/L.The sensor showed good selectivity and demonstrated high accuracy for the analysis of 4-nitrophenol and cerium(IV)in actual water samples.

关键词： Carbon dots Fluorescence sensor 4-Nitrophenol Cerium(IV) Water samples

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Bioorthogonal microglia-inspired mesenchymal stem cell bioengineering system creates livable niches for enhancing ischemic stroke recovery via the hormesis

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Acta Pharmaceutica Sinica B 2024年第3期14卷 1412-1427页

作者： Jianpei Xu Yinzhe Sun Yang You Yuwen Zhang Dan Huang Songlei Zhou Yipu Liu Shiqiang Tong Fenfen Ma Qingxiang Song Chengxiang Dai Suke Li Jigang Lei Zhihua Wang Xiaoling Gao Jun Chen shanghai Pudong Hospital&Department of Pharmaceutics School of PharmacyFudan UniversityShanghai 201203China Key Laboratory of Smart Drug Delivery Ministry of EducationSchool of PharmacyFudan UniversityShanghai 201203China Department of Pharmacology and Chemical Biology State Key Laboratory of Oncogenes and Related GenesShanghai Universities Collaborative Innovation Center for Translational MedicineShanghai Jiao Tong University School of MedicineShanghai 200025China Department of Emergency Shanghai Pudong HospitalFudan University Pudong Medical CenterShanghai 201399China Institute of science and technology for Brain-Inspired Intelligence&Department of Neurology Fudan UniversityShanghai 201203China Department of Rehabilitation Medicine Huashan HospitalFudan UniversityShanghai 201203China Daxing Research Institute University of Science and Technology BeijingBiomedical Industry BaseZhongguancun Science and Technology ParkBeijing 102600China Cellular Biomedicine Group Inc. Shanghai 201210China

Mesenchymal stem cells(MSCs)experience substantial viability issues in the stroke infarct region,limiting their therapeutic efficacy and clinical translation.High levels of deadly reactive oxygen radicals(ROS)and proinflammatory cytokines(PC)in the infarct milieu kill transplanted MSCs,whereas low levels of beneficial ROS and PC stimulate and improve engrafted MSCs’viability.Based on the intrinsic hormesis effects in cellular biology,we built a microglia-inspired MSC bioengineering system to transform detrimental high-level ROS and PC into vitality enhancers for strengthening MSC therapy.This system is achieved by bioorthogonally arming metabolic glycoengineered MSCs with microglial membrane-coated nanoparticles and an antioxidative extracellular protective layer.In this system,extracellular ROSscavenging and PC-absorbing layers effectively buffer the deleterious effects and establish a microlivable niche at the level of a single MSC for transplantation.Meanwhile,the infarct’s inanimate milieu is transformed at the tissue level into a new living niche to facilitate healing.The engineered MSCs achieved viability five times higher than natural MSCs at seven days after transplantation and exhibited a superior therapeutic effect for stroke recovery up to 28 days.This vitality-augmented system demonstrates the potential to accelerate the clinical translation of MSC treatment and boost stroke recovery.

关键词： Ischemic stroke Mesenchymal stem cell Cell engineering Hormesis effect Bioorthogonal chemistry Microglia Reactive oxygen spices Proinflammatory cytokines

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Multifunctional RGD coated a single-atom iron nanozyme:A highly selective approach to inducing ferroptosis and enhancing immunotherapy for pancreatic cancer

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Nano Research 2024年第6期17卷 5469-5478页

作者： Haoqi Pan Xu Chen Mingming Xiao He Xu Jiansheng Guo Zhiyi Lu Dong Cen Xianjun Yu Si Shi Department of Pancreatic Surgery Fudan University Shanghai Cancer CenterShanghai 200032China Department of Oncology Shanghai Medical CollegeFudan UniversityShanghai 200032China shanghai Pancreatic Cancer Institute Shanghai 200032China Pancreatic Cancer Institute Fudan UniversityShanghai 200032China Key Laboratory of Advanced Fuel Cells and Electrolyzers technology of Zhejiang Province Qianwan Institute of CNITECHNingbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China Department of Pathology of Sir Run Run Shaw Hospital Zhejiang University School of MedicineHangzhou 310016China Key Laboratory of Laparoscopic technology of Zhejiang Province Department of General SurgerySir Run Run Shaw HospitalZhejiang University School of MedicineHangzhou 310016China

Nanozyme is a new promising approach to cancer therapy for its ability to induce ferroptosis by activating H_(2)O_(2)via a traditional radical pathway and enhance cancer immunotherapy.However,short half-life period of hydroxyl radical(·OH)results in unsatisfied effectiveness.Herein,we synthesized a single-atom iron nanozyme(Fe-SAzyme),which can activate H_(2)O_(2)via a non-radical pathway to generate Fe-based reactive oxygen species(ROS)(O=FeO_(3)=O)for promoting the ferroptosis of pancreatic cancer cells.This Fe-SAzyme could be specifically phagocytosed by pancreatic cancer cells,increasing ROS levels and inhibiting glutathione(GSH)synthesis,which activates ferroptosis.Tumor magnetic resonance imaging(MRI)showed decreased T2 signal after intravenous injection of RGD@Fe-AC(AC=activated carbon).Moreover,RGD@Fe-AC promoted dendritic cell(DC)maturation,overcame Treg-mediated immunosuppression,activated T cells to trigger adaptive immune responses,and enhanced the efficacy ofα-PD-L1 immunotherapy.Our research demonstrated that RGD@Fe-AC provided a straightforward,easily implemented,and selective approach for pancreatic cancer treatment and immunotherapy.

关键词： single-atom iron nanozyme pancreatic cancer immunotherapy ferroptosis

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Reduced expression of semaphorin 3A in osteoclasts causes lymphatic expansion in a Gorham-Stout disease(GSD)mouse model

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Journal of Zhejiang University-science B(Biomedicine & Biotechnology) 2024年第1期25卷 38-50页

作者： Dongfang ZHANG Hao XU Chi QIN Kangming CAI Jing ZHANG Xinqiu XIA Jingwen BI Li ZHANG Lianping XING Qianqian LIANG Wensheng WANG Laboratory of Molecular Medicine College of Life Science and State Key Laboratory of Cell Differentiation and RegulationHenan Normal UniversityXinxiang453007China Longhua Hospital&Spine Institute Shanghai University of Traditional Chinese MedicineShanghai200032China Key Laboratory of Theory and Therapy of Muscles and Bones Ministry of Education(Shanghai University of Traditional Chinese Medicine)Shanghai201203China Department of Pathology and Laboratory Medicine University of Rochester Medical CenterRochester14642USA

Gorham-Stout disease(GSD)is a sporadic chronic disease characterized by progressive bone dissolution,absorption,and disappearance along with lymphatic vessel infiltration in bone-marrow cavities.Although the osteolytic mechanism of GSD has been widely studied,the cause of lymphatic hyperplasia in GSD is rarely investigated.In this study,by comparing the RNA expression profile of osteoclasts(OCs)with that of OC precursors(OCPs)by RNA sequencing,we identified a new factor,semaphorin 3A(Sema3A),which is an osteoprotective factor involved in the lymphatic expansion of GSD.Compared to OCPs,OCs enhanced the growth,migration,and tube formation of lymphatic endothelial cells(LECs),in which the expression of Sema3A is low compared to that in OCPs.In the presence of recombinant Sema3A,the growth,migration,and tube formation of LECs were inhibited,further confirming the inhibitory effect of Sema3A on LECs in vitro.Using an LEC-induced GSD mouse model,the effect of Sema3A was examined by injecting lentivirus-expressing Sema3A into the tibiae in vivo.We found that the overexpression of Sema3A in tibiae suppressed the expansion of LECs and alleviated bone loss,whereas the injection of lentivirus expressing Sema3A short hairpin RNA(shRNA)into the tibiae caused GSD-like phenotypes.Histological staining further demonstrated that OCs decreased and osteocalcin increased after Sema3A lentiviral treatment,compared with the control.Based on the above results,we propose that reduced Sema3A in OCs is one of the mechanisms contributing to the pathogeneses of GSD and that expressing Sema3A represents a new approach for the treatment of GSD.

关键词： Semaphorin 3A Gorham-Stout disease Osteoclast Osteolysis Lymphatic endothelial cell

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Elevated peripheral levels of receptor-interacting protein kinase 1(RIPK1)and IL-8 as biomarkers of human amyotrophic lateral sclerosis

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Signal Transduction and Targeted Therapy 2024年第1期9卷 271-278页

作者： Jun Wei Min Li Zhi Ye Xinqian Hu Xiaoyan He Jia Wang Gaofeng Chen Chengyu Zou Daichao Xu Hongbing Zhang Junying Yuan Yunhong Zha Institute of Neural Regeneration and Repair and Department of Neurology The First College of Clinical Medical ScienceYichang Central HospitalCollege of Basic Medical ScienceChina Three Gorges UniversityHubei Province Clinical Medical Research Center for Rare Diseases of Nervous SystemYichang 443000China Interdisciplinary Research Center on Biology and Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai Key Laboratory of Aging StudiesShanghai 201210China State Key Laboratory of Common Mechanism Research for Major Diseases Haihe Laboratory of Cell EcosystemDepartment of PhysiologyInstitute of Basic Medical Sciences and School of Basic MedicineChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijingChina

Amyotrophic lateral sclerosis(ALS)is a devastating fatal neurodegenerative disease with no cure.Receptor-interacting protein kinase 1(RIPK1)has been proposed to mediate pathogenesis of ALS.Primidone has been identified as an old drug that can also inhibit RIPK1 kinase.We conducted a drug-repurposing biomarker study of primidone as a RIPK1 inhibitor using SOD1G93A mice and ALS patients.SOD1G93A mice treated with primidone showed significant delay of symptomatic onset and improved motor performance.One-hundred-sixty-two ALS participants dosed daily with primidone(62.5 mg)completed 24-week follow-up.A significant reduction was showed in serum levels of RIPK1 and IL-8,which were significantly higher in ALS patients than that of healthy controls(P<0.0001).Serum RIPK1 levels were correlated positively with the severity of bulbar symptoms(P<0.05).Our study suggests that serum levels of RIPK1 and IL-8 in peripheral can be used as clinical biomarkers for the activation of RIPK1 in central nervous system in human ALS patients.Repurposing primidone may provide a promising therapeutic strategy for ALS.The effect of primidone for the treatment of other inflammatory diseases may also be considered,since the activation of RIPK1 has been implicated in mediating a variety of inflammatory diseases including COVID-19-associated cytokine release syndrome(CRS).(ChiCTR2200060149).

关键词： RIPK1 diseases Serum

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Photocatalytic vinyl radical-mediated multicomponent 1,4-/1,8-carboimination across alkynes and olefins/(hetero)arenes

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science China Chemistry 2024年第2期67卷 558-567页

作者： Shan-Shan Li Yu-Shi Jiang Xue-Ling Luo Xuming Ran Yuqiang Li Dong Wu Cheng-Xue Pan Peng-Ju Xia School of Chemistry and Pharmaceutical sciences Guangxi Normal UniversityGuilin541004China shanghai Artificial Intelligence Laboratory Shanghai200433China The Institute for Advanced Studies Wuhan UniversityWuhan430064China

We developed a highly selective and efficient multicomponent transformation by utilizing alkynes and olefins/(hetero)arenes through photoinduced energy-transfer catalysis.The reaction involves the formation of three distinct chemical bonds,namely C(sp~3)–C(sp~2),C(sp~2)–C(sp~3),and C(sp~3)–N,in a single coordinated manner.The strategy used a vinyl radical-mediated radical relay approach under mild conditions,exhibiting a broad substrate scope(>70 examples),excellent functional-group tolerance,and remarkable regio-and anti-stereoselectivity.Through the utilization of a combination of experimental techniques and density functional theory(DFT),we delved deeper into the mechanistic intricacies of this distinctive system.Results revealed that the selective radical addition to electron-deficient alkynes,rather than olefins,was governed by the inherent reactivity of alkyl radicals.This discovery presented a highly effective approach for the synthesis of stereodefined multisubstituted alkenes.

关键词： alkyne-olefin coupling DFT studies regio-and anti-stereoselectivity multisubstituted alkenes

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