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Molecular Engineering of Aptamer to Solubilize Hydrophobic Near-Infrared Photosensitizer for Enhanced Cancer Photodynamic Therapy

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CCS Chemistry 2024年第5期6卷 1240-1254页

作者： Rongjun Zhang Ding-Kun ji Defan Yao Zeyu xiao Weihon. Tan Institute of Molecular Medicine(IMM) Renji HospitalState Key Laboratory of Oncogenes and Related GenesShanghai Jiao Tong University School of MedicineShanghai 200240 Department of Radiology Xinhua HospitalShanghai Jiao Tong University School of MedicineShanghai 200092 Department of Pharmacology and Chemical Biology School of MedicineShanghai Jiao Tong UniversityShanghai 200025 Zhejiang Cancer Hospital Hangzhou Institute of Medicine(HIM)The Chinese Academy of SciencesHangzhouZhejiang 310022 Molecular Science and Biomedicine Laboratory(MBL) State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollege of BiologyAptamer Engineering Center of Hunan ProvinceHunan UniversityChangshaHunan 410082

Photodynamic therapy(PDT)is a clinically representative treatment strategy for ***,conventional photosensitizers(PSs)are usually hampered by poor water solubility and low targeting ***,we report the precise molecular engineering of aptamer oligonucleotides to solubilize hydrophobic near-infrared(NIR)PSs for enhanced cancer *** pyropheophorbide A(PA)is precisely conjugated to aptamer oligonucleotides by combing DNA solid-phase synthesis technology and Cu-free click *** coupling of insoluble PA to hydrophilic aptamer oligonucleotides vastly improves its solubility to as high as 750μM in water without any cosolvent,resulting in an enhanced NIR fluorescence property(quantum yield=23%)and ***,the targeting ability of aptamer oligonucleotides is not affected by our molecular engineering *** reactive oxygen species(ROS)are produced intracellularly with 660 nm laser irradiation,eliciting mitochon.ria damage and cell *** growth is effectively inhibited with a single dose of aptamer-PA conjugates without in vivo *** therapeutic effect is more than 20-fold higher than that of *** with traditional formulation,using aptamer oligonucleotides as functional carriers to solubilize hydrophobic NIR PSs is more precise and *** DNA molecular engineering strategy paves a way for the rational design of molecularly targeted medicine for future clinical cancer therapy.

关键词： aptamer aptamer-drug conjugates photosensitive drugs targeted photodynamic therapy cancer theranostics

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Lactonization of dyes promoted by a coordination cage facilitates cavity-induced chromism as ion mobile detector

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Science China Chemistry 2024年第5期67卷 1554-1560页

作者： Liangliang Zhang Yu Liang Zhifeng xiao Yuxuan Meng jinyi Huang Xi Lin ji Li hon.-Cai Zhou Yu Fang Strait Institute of Flexible Electronics(SIFE Future Technologies)Fujian Normal University and Strait Laboratory of Flexible Electronics(SLoFE)Fuzhou 350017China State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Chemistry Texas A&M UniversityCollege StationTexas 77842-3012USA State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Frontiers Science Center for Flexible Electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KLoFE)Northwestern Polytechnical UniversityXi’an 710072China

Dye molecules often change colors(so-called “chromism”) according to the environment variation. However, they are rarely induced by a catalytic amount of cavity. Through encapsulation in the cavity of a porous coordination cage(PCC-2), Rhodamine B(1) is transformed from red quinonoid form(1q) into colorless lactone form(1l) in aprotic polar solutions. The μ4-OH groups in the cavity of PCC-2 are shown to stabilize the uncommon zwitterion intermediate(1z), followed by converting to 1l, thus accelerating the equilibrium. The chromism is catalyzed by 0.25 mol% of PCC-2, and the reaction rate is improved by 80,400times. 1@PCC-2 can be further fabricated to a sol-gel that exhibits ion recognition properties. The resulting encapsulation and stabilization of an unconventional intermediate by a catalytic amount of the coordination cage provides fundamental insights into molecular isomerization and has potential use in chemical sensing.

关键词： porous coordination cage Zwitterion intermediate cavity Rhodamine B chromism

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang jin-Ting Wu jian Gao ji-Jun Zou xiao-Dong Zhu State Key Laboratory Base of Eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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Effects of cooling rate on microstructure and microhardness of directionally solidified Galvalume alloy

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China Foundry 2024年第3期21卷 213-220页

作者： ji-peng Li De-gao Qiao jian Li xiao-yang Luo Peng Peng Xian-tao Yan Xu-dong Zhang Gansu jiu Steel Group hon.xing Iron and Steel Co. Ltd.Jiayuguan 735111GansuChina School of Materials and Energy Lanzhou UniversityLanzhou 730000China

The influences of cooling rate on the phase constitution,microstructural length scale,and microhardness of directionally solidified Galvalume(Zn-55Al-1.6Si)alloy were investigated by directional solidification experiments at different withdrawal speeds(5,10,20,50,100,200,and 400μm·s^(-1)).The results show that the microstructure of directionally solidified Galvalume alloys is composed of primary Al dendrites,Si-rich phase and(Zn-Al-Si)ternary eutectics at the withdrawal speed ranging from 5 to 400μm·s^(-1).As the withdrawal speed increases,the segregation of Si element intensifies,resulting in an increase in the area fraction of the Si-rich *** addition,the primary Al dendrites show significant refinement with an increase in the withdrawal *** relationship between the primary dendrite arm spacing(λ_(1))and the thermal parameters of solidification is obtained:λ_(1)=127.3V^(-0.31).Moreover,as the withdrawal speed increases from 5 to 400μm·s^(-1),the microhardness of the alloy increases from 90 HV to 151 *** is a combined effect of grain refinement and second-phase strengthening.

关键词： Galvalume alloy directional solidification microstructure length scale microhardness

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The Effect and Mechanism of Fructus lycii on Improvement of Exercise Fatigue Using a Network Pharmacological Approach with in vitro Experimental Verification

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Biomedical and Environmental Sciences 2024年第1期37卷 42-53页

作者： ji xiao Ning LIU Zhao Ping ZHANG Chao Zheng CHEN Min LIANG jiang LU jiang ZHANG Lei National Resource Center for Chinese Materia Medica China Academy of Chinese Medical SciencesBeijing 100700China China National Center for Food Safety Risk Assessment Beijing 100022China Chinese Center for Disease Control and Prevention Beijing 102206China

Objective This study aimed to investigate the effect and underlying mechanism of Fructus lycii in improving exercise *** A network pharmacological approach was used to explore potential mechanisms of action of Fructus *** muscle C2C12 cells and immunofluorescence were employed to verify the effect and mechanism of the representative components in Fructus lycii predicted by network pharmacological *** Six potential active components,namely quercetin,β-sitosterol,stigmasterol,7-Omethylluteolin-6-C-beta-glucoside_qt,atropine,and glycitein,were identified to have potency in improving exercise fatigue via multiple pathways,such as the PI3K-Akt,neuroactive ligand-receptor interaction,IL-17,TNF,and MAPK signaling *** immunofluorescence results indicated that quercetin,a significant active component in Fructus lycii,increased the mean staining area of 2-NBDG,TMRM,and MitoTracker,and decreased the area of CellRox compared to the ***,the protein expression levels of p-38 MAPK,p-MAPK,p-JNK,p-PI3K,and p-AKT markedly increased after quercetin *** Fructus lycii might alleviate exercise fatigue through multiple components and *** these,quercetin appears to improve exercise fatigue by enhancing energy metabolism and reducing oxidative *** PI3K-AKT and MAPK signaling pathways also appear to play a role in this process.

关键词： Fructus lycii Exercise fatigue Network pharmacology

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No Incidence of Liver Cancer Was Observed in A Retrospective Studyof Patients with Aristolochic Acid Nephropathy

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Chinese Journal of Integrative Medicine 2024年第2期30卷 99-106页

作者： SU Tao FANG Zhi-e GUO Yu-ming WANG Chun-yu WANG jia-bo ji Dong BAI Zhao-fang YANG Li xiao xiao-he Renal Division Department of MedicinePeking University First HospitalBeijing(100034)China Department of Pharmacy Chongqing Hospital of Traditional Chinese MedicineChongqing(400021)China Department of Hepatology Fifth Medical Center of Chinese PLA General HospitalBeijing(100039)China China Military Institute of Chinese Materia Fifth Medical Center of Chinese PLA General HospitalBeijing(100039)China Phase I Clinical Trials Unit Department of Medicine for Infectious DiseasesFifth Medical Center of Chinese PLA General HospitalBeijing(100039)China Department of Pharmacy Affiliated Hospital of Shandong University of Traditional Chinese MedicineJinan(250000)China National Key Laboratory of Kidney Diseases Beijing(100039)China

Objective:To assess the risk of aristolochic acid(AA)-associated cancer in patients with AA nephropathy(AAN).Methods:A retrospective study was conducted on patients diagnosed with AAN at Peking University First Hospital from January 1997 to December ***-term surveillance and follow-up data were analyzed to investigate the influence of different factors on the prevalence of *** primary endpoint was the incidence of liver cancer,and the secondary endpoint was the incidence of urinary cancer during 1 year after taking AA-containing medication to ***:A total of 337 patients diagnosed with AAN were included in this *** the initiation of taking AA to the termination of follow-up,39 patients were diagnosed with *** cases of liver cancer were observed throughout the entire follow-up period,with urinary cancer being the predominant type(34/39,87.17%).Logistic regression analysis showed that age,follow-up period,and diabetes were potential risk factors,however,the dosage of the drug was not significantly associated with urinary ***:No cases of liver cancer were observed at the end of ***,a high prevalence of urinary cancer was observed in AAN *** a direct causality between AA and HCC is challenging.

关键词： aristolochic acid hepatocellular carcinoma urinary cancer drug safety retrospective study

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Artemsieverolactones A—H,Eight Guaiane-Type Sesquiterpenoid Trimers from Artemisia sieversiana

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Chinese Journal of Chemistry 2024年第10期42卷 1084-1092页

作者： Wei Dong xiao-Yan Huang Tian-Ze Li Yan-Mei Weng Chang-An Geng ji-Jun Chen State Key Laboratory of Phytochemistry and Plant Resources in West China Kunming Institute of BotanyChinese Academy of SciencesKunmingYunnan 650201China University of Chinese Academyof Sciences Beijing 100049China

Eight new guaiane-type sesquiterpenoid trimers,artemsieverolactones A—H,possessing unprecedented scaffolds via biocatalyzed[4+2]Diels−Alder cycloaddition reactions were identified from Artemisia *** structures were determined by comprehensive spectroscopic data,single-crystal X-ray diffraction analyses,and ECD *** terms of structure,artemsieverolactones A—H are first examples of sesquiterpenoid trimers from guaiane-type sesquiterpenoid through four different[4+2]Diels−Alder cycloaddition *** fibrosis assay suggested that five compounds exhibited activity against HSC-LX2 with IC_(50)values ranging from 37.8 to 117.1μmol/*** most active artemsieverolactone B(2)displayed significant inhibitory activity against HSC-LX2 with IC_(50)value of 37.8μmol/L,which was 3 times more active than the positive drug silybin(IC_(50),139.7μmol/L).Preliminary mechanism study revealed that artemsieverolactone B could inhibit the deposition of human collagen typeⅠ(ColⅠ),human hyaluronic acid(HA),and human laminin(HL)with IC_(50)values of 40.4μmol/L(Col I),55.1μmol/L(HL),47.3μmol/L(HA),which was 2 to 3-fold more potent than silybin.

关键词： Artemisia sieversiana Artemsieverolactones A-H Guaiane-type sesquiterpenoid trimers Antihepatic fibrosis Extracellular matrix Cancer NMR spectroscopy X-ray diffraction

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Molecular docking-aided AIEgen design: concept, synthesis and applications

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Science China Chemistry 2024年第8期67卷 2614-2628页

作者： jian-Qing Zhang xiao-Yu Xu Fu-Sheng Liu Shu-Qiang Cao Yu-Xin Gui Yi-Wen Su xiao-Yu He ji-Yuan Liang You-Quan Zou Department of Radiation and Medical Oncology Zhongnan Hospital of Wuhan UniversitySchool of Pharmaceutical SciencesWuhan UniversityWuhan 430071China Key Laboratory of Combinatorial Biosynthesis and Drug Discovery Ministry of EducationWuhan UniversityWuhan 430071China Tai Kang Center for Life and Medical Sciences Wuhan UniversityWuhan 430071China Department of Hepatobiliary Pancreatic SurgeryZhongnan Hospital of Wuhan UniversityWuhan 430071China

Aggregate-induced emission luminogens(AIEgens) have been widely used in biological imaging, chemical sensing, and disease treatments. The rational design and construction of AIEgens have received considerable research interests during the last few years. Herein, molecular docking-aided AIEgen design has been reasonably proposed and AIEgen TBQZY with excellent ~1O_(2) generation ability has been synthesized. The newly developed TBQZY could efficiently kill S. epidermidis and methicillinresistant S. epidermidis(MRSE) by tightly binding to bacteria and triggering the accumulation of ~1O_(2) in bacteria. TBQZY specifically regulated the immune system and polarized macrophages from M1 to M2 to accelerate the elimination of biofilm in vivo. In addition, healing acceleration was observed in chronic wounds treated with TBQZY, and side effects were ***, TBQZY had extraordinary potential for combating drug-resistant bacteria in the clinical setting. This research not only provided new concepts for the design of AIEgens, but also shed some lights on the discovery of drugs against drug-resistant bacteria.

关键词： AIEgen molecular docking drug-resistant bacteria biofilm chronic wounds healing

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Review of Iron-Based Catalysts for Carbon Dioxide Fischer-Tropsch Synthesis

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Transactions of Tianjin University 2024年第2期30卷 178-197页

作者： ji-Yue jia Yu-Ling Shan Yong-xiao Tuo Hao Yan Xiang Feng De Chen State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao 266580China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China Department of Chemical Engineering Norwegian University of Science and Technology7491 TrondheimNorway

Capturing and utilizing CO_(2)from the production process is the key to solving the excessive CO_(2)emission problem. CO_(2)hydrogenation with green hydrogen to produce olefins is an effective and promising way to utilize CO_(2)and produce valuable chemicals. The olefins can be produced by CO_(2)hydrogenation through two routes, i.e., CO_(2)-FTS (carbon dioxide Fischer- Tropsch synthesis) and MeOH (methanol-mediated), among which CO_(2)-FTS has significant advantages over MeOH in practical applications due to its relatively high CO_(2)conversion and low energy consumption potentials. However, the CO_(2)-FTS faces challenges of difficult CO_(2)activation and low olefins selectivity. Iron-based catalysts are promising for CO_(2)-FTS due to their dual functionality of catalyzing RWGS and CO-FTS reactions. This review summarizes the recent progress on iron-based catalysts for CO_(2)hydrogenation via the FTS route and analyzes the catalyst optimization from the perspectives of additives, active sites, and reaction mechanisms. Furthermore, we also outline principles and challenges for rational design of high-performance CO_(2)-FTS catalysts.

关键词： CO_(2)hydrogenation Olefins CO_(2)-FTS Iron-based catalysts

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Regulable toehold lock for the effective control of strand displacement reaction sequence and circuit leakage

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Chinese Chemical Letters 2024年第7期35卷 372-376页

作者： Kuangdi Luo Yang Qin Xuehao Zhang Hanxu ji Heao Zhang jiangtian Li Xianjin xiao Xinyu Wang Department of Breast Surgery Second Hospital of Jilin UniversityChangchun 130041China Institute of Reproductive Health Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China Department of Laboratory Medicine Tongji HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China Department of Pancreatic Surgery Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China School of Life Science and Technology Wuhan Polytechnic UniversityWuhan 430023China

Strand displacement reaction enables the construction of enzyme-free DNA reaction networks,thus has been widely applied to DNA circuit and *** has the characteristics of high efficiency,universality and ***,the existing regulation tools cannot enable effective control of the reaction sequence,which undoubtedly limits the construction of complex nucleic acid ***,we developed a regulation tool,toehold lock,and achieved strict control of reaction sequence without loss of the main reaction signal ***,we applied the tool to scenarios such as seesaw circuits,AND/OR logic gates,and entropy-driven circuits,and respectively demonstrated its significant superiority compared to the original *** believe that the proposed toehold lock has greatly optimized the efficiency of DNA strand displacement-based networks,and we anticipate that the tool will be widely used in multiple fields.

关键词： DNA circuit Toehold lock DNA strand displacement Reaction sequence Seesaw circuit

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