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MOF-based magnetic microrobot swarms for pH-responsive targeted drug delivery

Science China Chemistry 2024年第4期67卷 1216-1223页

作者： Qinyi Cao Yifan Zhang Yanping Tang Changjin Wu Jizhuang Wang Dan Li College of Chemistry and Materials Science Jinan UniversityGuangzhou 510632China Guangdong Provincial Key Laboratory of Functional Supramolecular coordination Materials and Applications Jinan UniversityGuangzhou 510632China Guangdong Provincial Key Laboratory of Spine and Spinal Cord Reconstruction The Fifth Affiliated Hospital(Heyuan Shenhe People’s Hospital)Jinan UniversityHeyuan 517000China JNU-HKUST Joint Laboratory for Neuroscience and Innovative Drug Research College of PharmacyJinan UniversityGuangzhou 510632China Department of Chemistry The University of Hong KongHong KongChina

Metal-organic frameworks(MOFs)hold significant potential as vehicles for drug delivery due to their expansive specific surface area,biocompatibility,and versatile ***,magnetically actuated micro/nano-robots(MNRs)offer distinct advantages,such as untethered and precise *** fusion of these technologies presents a promising avenue for achieving non-invasive targeted drug ***,we report a MOF-based magnetic microrobot swarm(MMRS)for targeted *** approach overcomes limitations associated with a single MNR,including limited drug loading and the risk of loss during *** select Zeolitic Imidazolate Framework-8(ZIF-8)as the drug vehicle for its superior loading potential and p H-sensitive *** design incorporates magnetic responsive components into the one-pot synthesis of Fe@ZIF-8,enabling collective behaviors under *** the yaw angle of alternating magnetic fields and nanoparticles'amount,the MMRSs with controllable size achieve instantaneous transformation among different configurations,including vortex-like swarms,chain-like swarms,and elliptical swarms,facilitating adaptation to environmental *** to the subcutaneous T24 tumor site,the MMRSs with encapsulated doxorubicin(DOX)automatically degrade and release the drug,leading to a dramatic reduction of the tumor in *** investigation signifies a significant advancement in the integration of biodegradable MOFs into microrobot swarms,ushering in new avenues for accurate and non-invasive targeted drug delivery.

关键词： magnetic microrobot swarm MOF nanoparticles magnetic propulsion pH-responsive drug release targeted drug delivery

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Selenium-engineered bottom-up-synthesized lanthanide coordination nanoframeworks as efficiency X-ray-responsive radiosensitizers

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Nano Research 2023年第4期16卷 5169-5175页

作者： Liwen Zhu Leung Chan Junping Wang Mingkai Chen Fei Cai Yuan Tian Li Ma Tianfeng Chen Department of Chemistry and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Radiotherapy is one of the main therapeutic methods for cancers;however,nonselective killing of normal cells and tumor cells by X-ray inevitably results in toxicity and side *** low-toxicity and high-efficiency radiosensitizers to reduce the practical dose of X-ray is a promising approach to overcoming these side ***,we report the use of carboxylatecontaining organic ligands to construct one-dimensional high-Z lanthanide chains for efficient response to *** onedimensional lanthanide chains are stacked through weak interactions to form coordination nanoframeworks in the presence of polyethylenimine(PEI).The morphology and activity of the synthesized nanoframeworks can be regulated through selenium atom *** study presents a promising approach for effective radiotherapy through selenium-engineering stable lanthanide nanoframeworks with precise coordination structures as radiosensitizers to mitigate X-ray side effects.

关键词： selenium lanthanide coordination nanoframeworks radiotherapy radiosensitizers

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Metal-organic frameworks as photocatalysts for aerobic oxidation reactions

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Science China Chemistry 2023年第6期66卷 1634-1653页

作者： Kun Wu Xin-Yi Liu Pei-Wen Cheng Mo Xie Weigang Lu Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Metal-organic frameworks(MOFs)are emerging as one of the most intriguing classes of heterogeneous photocatalysts owing to their abundant structures,tunable porosity,and versatile *** advantages of bottom-up design and reticular synthesis render MOF materials with desired photocatalytic properties for targeted *** this review,we discussed the design and synthesis of MOF-based photocatalysts as well as strategies for enhancing photocatalytic *** progress on MOFs as platforms for photocatalytic aerobic oxidation reactions was summarized and categorized according to the types of bond *** hope this review will give an in-depth insight into MOF-based photocatalytic systems for not only aerobic oxidation reactions but also other organic transformations.A brief outlook on the challenges and opportunities of MOFs as heterogeneous photocatalysts is provided at the end of the review.

关键词： metal-organic frameworks heterogeneous photocatalyst reactive oxygen species aerobic oxidation organic synthesis

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Identification of galectin-3 as a novel potential prognostic/predictive biomarker and therapeutic target for cerebral cavernous malformation disease

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Genes & Diseases 2024年第1期11卷 67-71页

作者： Souvik Kar Andrea Perrelli Kiran Kumar Bali Raffaella Mastrocola Arpita Kar Bushra Khan Luis Gand Arnab Nayak Christian Hartmann Wolfram SKunz Amir Samii Helmut Bertalanffy Saverio Francesco Retta International Neuroscience Institute Rudolf-PichlmayrStrasse 4Hannover 30625Germany Department of Clinical and Biological Sciences University of TorinoOrbassano(TO)10043Italy CCM Italia Research Network National Coordination Center at the Department of Clinical and Biological SciencesUniversity of TorinoOrbassano(TO)10043Italy Department of Experimental Pain Research Mannheim Center for Translational Neuroscience(MCTN)Medical Faculty MannheimHeidelberg UniversityMannheim 68167Germany Department of Kidney Liver and Metabolic DiseasesChildren’s HospitalHannover Medical SchoolHannover 30625Germany Ricarda-Huch-Street-10B Hannover 30880Germany Institute of Molecular and Cell Physiology Hannover Medical SchoolHannover 30625Germany Department of Neuropathology Institute of PathologyHannover Medical SchoolHannover 30625Germany Institute of Experimental Epileptology and Cognition Research and Department of Epileptology University Hospital BonnVenusberg-Campus 1Bonn 53127Germany epartment of Pharmacology and Physiology University of Rochester Medical CenterRochesterNY 14642USA

cerebrovascular disease of genetic origin characterized by abnormally dilated capillaries and a wide spectrum of symptoms,including headaches,seizures,neurological deficits,and intracerebral *** unpredictable clinical course and the current lack of therapies make the identification of prognostic and predictive biomarkers an imperative research challenge.1 Herein,we provide evidence that galectin-3(Gal-3),a major tissue and circulating biomarker of oxidative stress and inflammation,is significantly up-regulated both in CCM patients and ***,wholetranscriptome sequencing,qRT-PCR,and Western blotting studies demonstrated a significant up-regulation of Gal-3 expression levels both in surgical CCM specimens and in blood samples of CCM patients.

关键词： inflammation cerebral dilated

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An anthraquinone-based Cu(I) cyclic trinuclear complex for photo-catalyzing C–C coupling reactions

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Science China Chemistry 2023年第12期66卷 3525-3531页

作者： Yu-Mei Wang Kai-Ming Mo Xiao Luo Ri-Qin Xia Jing-Yi Song Guo-Hong Ning Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Development of transition metal-based photocatalysts with low cost, strong visible light absorption, and high efficiency is a longstand pursuit for advanced organic synthesis, yet remains highly challenging. In this article, an anthraquinone-based copper(I)cyclic trinuclear complex(1) was designed and it featured strong visible light absorption, high charge separation efficiency and photochemical properties. Complex 1 as a heterogeneous photocatalyst can efficiently catalyze homo-coupling of terminal alkynes and denitrification-oxidative coupling reaction between hydrazinopyridine and terminal alkynes with excellent yield(up to 99%), broad substrate tolerance(27 examples) and superior reusability(up to 10 cycles without loss of performance) under mild conditions.

关键词： cyclic trinuclear complex photocatalysis C–C coupling reaction

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Designing anticancer combretastatin A-4 analogues with aggregation-induced emission characteristics

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Science China Chemistry 2022年第4期65卷 694-698页

作者： Rucheng Zhao Yusheng Wu Yuequn Zhang Jiabao Ling Xinxin Liu Jiaqi Xiang Xiangchao Zeng Tianfeng Chen College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Herein a series of combretastatin A-4(CA-4)analogues with aggregation-induced emission characteristics(compounds a1-a19)were rationally designed and *** research results showed that the mechanism of AIE of a1-a19 could be attributed to the dual function of the restriction of intramolecular motion(RIM)and J-aggregate ***,the detailed investigation on the action mechanisms revealed that a19 diffused from lysosomes into the cytoplasm,and then targeted the colchicine binding site to induce cell cycle arrest and apoptosis in cancer *** results provide new ideas and impetus for the rational design of CA-4 analogues.

关键词： combretastatin A-4 analogues anticancer AIE carbazole fluorene

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Fabricating multi-porous carbon anode with remarkable initial coulombic efficiency and enhanced rate capability for sodium-ion batteries

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Chinese Chemical Letters 2023年第1期34卷 127-132页

作者： Yong Tong Yuanji Wu Zihao Liu Yongshi Yin Yingjuan Sun Hongyan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Due to the abundant sodium reserves and high safety,sodium ion batteries(SIBs)are foreseen a promising ***,hard carbon materials are very suitable for the anode of SIBs owing to their structure and cost ***,the unsatisfactory initial coulombic efficiency(ICE)is one of the crucial blemishes of hard carbon materials and the slow sodium storage kinetics also hinders their wide ***,with spherical nano SiO_(2)as pore-forming agent,gelatin and polytetrafluoroethylene as carbon sources,a multi-porous carbon(MPC)material can be easily obtained via a co-pyrolysis method,by which carbonization and template removal can be achieved synchronously without the assistance of strong acids or strong *** a result,the MPC anode exhibited remarkable ICE of 83%and a high rate capability(208 m Ah/g at 5 A/g)when used in sodium-ion half ***,coupling with Na3V2(PO4)3as the cathode to assemble full cells,the as-fabricated MPC//NVP full cell delivered a good rate capability(146 m Ah/g at 5 A/g)as well,implying a good application prospect the MPC anode has.

关键词： Multi-porous carbon Initial coulombic efficiency Rate capability Sodium ion batteries Silica template

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Self-assembly of a quadrangular prismatic covalent cage templated by zinc ions:A selective fluorescent sensor for palladium ions

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Chinese Chemical Letters 2023年第6期34卷 541-544页

作者： Ya-Liang Lai Hao-Jie Zhang Juan Su Xue-Zhi Wang Dong Luo Jia-Xing Liu Xiao-Ping Zhou Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Herein we report a covalent cage TPE-Zn_(4)based on a tetraphenylethylene molecule via subcomponent self-assembly,which is templated by zinc ***-Zn_(4)features a quadrangular prismatic cage structure,which is characterized by NMR,mass spectrum,and single-crystal X-ray ***-Zn_(4)emitted orange fluorescence(λ_(em)=620 nm)in DMSO solution under the irradiation of UV light(λ_(ex)=395 nm)and can be applied as a fluorescence sensor for selectively detecting Pd^(2+).The fluorescence of TPE-Zn_(4)was quenched by Pd^(2+)in DMSO solution,and a very low detection limit of 62.3 n M was *** studies reveal that the Pd^(2+)can replace the Zn^(2+),and the heavy atom effect and chelation-enhanced quenching effect between the Pd^(2+)and the cage probably cause the fluorescence quenching.

关键词： Subcomponent self-assembly Covalent cage Fluorescence sensor Detection of palladium ions Photoluminescence

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An Eosin Y Encapsulated Cu(Ⅰ)Covalent Metal Organic Framework for Efficient Photocatalytic Sonogashira Cross-coupling Reaction

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Chemical Research in Chinese Universities 2022年第2期38卷 415-420页

作者： YOU Peiye WEI Rongjia NING Guohong LI Dan College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632P.R.China

Sonogashira cross-coupling reaction is significant for the formation of C―C bonds and the creation of new substance in organic synthesis,which is usually catalyzed using noble metal,such as palladium or non-precious metal,such as copper under harsh reaction ***,we report the encapsulation of an organic dye(i.e.,Eosin Y,EY)into a Cu(I)cyclic trinuclear unit(CTU)based covalent-metal organic framework(CMOF),namely EY@JNM-1,which demonstrates outstanding photocatalytic performance for the Sonogashira cross-coupling reaction of iodobenzene with *** EY@JNM-1 not only exhibited high catalytic activity for the alkynes(>99%conversion)and excellent selectivity for the cross-coupling product(>99%)under mild conditions,but also displayed excellent stability and recyclability.

关键词： Covalent-metal organic framework Eosin Y Photocata-lysis Sonogashira cross-coupling reaction

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Structure of AcMet-Gly and Its Interaction with Palladium(II) Tetraaqua Complex Studied by Electrospray Mass Spectrometry and Density Functional Theory

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Chinese Journal of Chemistry 2004年第6期22卷 537-544页

作者：金晨张琳洪瑾杨高升朱龙根 State Key Laboratory of coordination Chemistry Coordination Chemistry Institute Nanjing University Nanjing Jiangsu 210093 China

The structure of dipepide AcMet-Gly was determined by X-ray crystallographic analysis. It possesses mono-clinic, space group P21 (No. 4), with cell dimensions of a=0.8571(2) nm, b=0.5871(2) nm, c=1.197(3) nm, =99.290(10), V=0.5944(15) nm3, Z=2, m=2.74 cm-1. Mononuclear chelates, described as [Pd(X)(S,N,O- AcMet-Gly)]+, in which Pd(II) is coordinated by thioether, deprotonated amide nitrogen, carbonyl oxygen of me-thionine and X (AcMetGly or other ligands present in aqueous solution or in mobile phase solution), were detected 5 min after mixing AcMet-Gly with [Pd(H2O)4]2+ at room temperature using electrospray ionization mass spectrometry. The geometry of [Pd(H2O)(S,N,O-AcMet-Gly)]+ is optimized at density functional B3LYP/LanL2DZ level. The fused five- and six-membered chelate is responsible for cleavage of Met-Gly bond. This is the first time to provide a direct evidence for Pd(II)-mediated cleavage of dipeptides via external solvent attack.

关键词： acetylmethionylglycine tetraaquapalladium(II) complex X-ray structure electrospray mass spec-trometry B3LYP density functional theory

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