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Self-assembly of a photoluminescent metal-organic cage and its spontaneous aggregation in dilute solutions enabling timedependent emission enhancement

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Science China Chemistry 2022年第6期65卷 1105-1111页

作者： Dong Luo Le-Xiong Wu Yan Zhang Yong-Liang Huang Xue-Ling Chen Xiao-Ping Zhou Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou510632China Department of Chemistry Shantou University Medical CollegeShantou515041China

Charged metal-organic cages generally produce aggregates with various morphologies and different properties through the multiple supramolecular interactions in solution. Herein, a luminescent hexahedral metal-organic cage containing pyrene chromophores is successfully constructed through coordination-driven subcomponent self-assembly. The cage exhibits novel spontaneous aggregation in a dilute solution and time-dependent luminescence enhancement behavior during the subsequent incubation process. Dynamic light scatter(DLS) and transmission electron microscopy(TEM) results prove that the metalorganic cages can form blackberry-like aggregates in methanol dilute solution. Unexpectedly, the luminescent intensity of this system shows a linear increase with the extension of the incubation time in methanol, and this process is also reflected in the change in the quantum yield of the system(2% to over 80% after 5 days incubation time). Ultraviolet-visible(UV-vis),1 H nuclear magnetic resonance(1 H NMR) and mass spectra show that metal-organic cages can stably exist in dilute solution. Timedepended DLS and TEM data reveal that the aggregates of metal-organic cages are gradually changed from the dense state to the loose one, which may involve the transition of the system from an energy unstable state to a stable one, probably leading to the unusual time-dependent luminescent property. This unique time-dependent luminescent cage aggregate can be potentially applied as a “supramolecular time meter”.

关键词： self-assembly metal-organic cage spontaneous aggregation time-dependent emission enhancement pyrene

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Porous metal-organic cage-based membranes

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Science China Chemistry 2023年第8期66卷 2169-2180页

作者： Lei Jia Xianhui Tang Yong Cui Yan Liu School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules and State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai200240China

As a new class of porous solid materials with structural variability,notable porosity,and good dispersibility,metal-organic cages(MOCs)have shown great promise as filler components for separation *** into MOC-based membranes has blossomed over the last decade because of their high performance in separation,desalination,and artificial *** this review,we summarize current membranes based on MOCs including mixed matrix membranes,cross-linked membranes,composite membranes,bilayer lipid membranes,and liquid membranes,and provide a brief overview of their *** challenges and opportunities in future developments are also discussed.

关键词： metal-organic cage membranes separation desalination artificial channels

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N-H Insertion Reactions Catalyzed by a Dirhodium metal-organic cage： A Facile and Recyclable Approach for C-N Bond Formation

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Chinese Journal of Chemistry 2017年第6期35卷 964-968页

作者： Jian Kang Lianfen Chen Hao Cui Li Zhang Cheng-Yong Su MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional Materials School of Chemistry Sun Yat-sen University Guangzhou Guangdong 510275 China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Shanghai 200032 China

A heterogeneous metal-organic cage based on Rh-Rh bonds [Rh4（pbeddb）4（H2O）2（DMAC）2] （MOC-18; pbeddb2- = 3,3＇-（1,3-phenylenebis（ethyne-2,1-diyl））dibenzoate） was applied to the N-- H insertion reactions wit... 详细信息

关键词： porous frameworks metal-organic cage heterogeneous catalysis C--N bond formation N--H inser-tion

Producing circularly polarized luminescence by radiative energy transfer from achiral metal-organic cage to chiral organic molecules

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Chinese Chemical Letters 2024年第8期35卷 498-502页

作者： Zhao-Xia Lian Xue-Zhi Wang Chuang-Wei Zhou Jiayu Li Ming-De Li Xiao-Ping Zhou Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China College of Chemistry and Chemical Engineering Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong ProvinceShantou UniversityShantou 515063China

The development of circularly polarized luminescence(CPL)materials with high performance is signifi-cantly ***,we develop a facial strategy for fabricating a CPL-active system by employing an achiral luminescent metal-organic cage(MOC)and chiral boron dipyrromethene(BODIPY)*** is achieved by taking advantage of the radiative energy transfer process,in which BODIPY molecules act as energy acceptors and MOCs act as *** CPL performance(maximum luminescence dissymme-try factor up to±1.5×10^(−3))can be tuned by adjusting the ratio between MOCs and ***-light emission with the CPL feature is obtained by using a ternary system including MOC,chiral BODIPY,and Rhodamine *** present work provides a facile and universal strategy to construct a CPL-active system by integrating achiral luminophores and chiral molecules.

关键词： Circularly polarized luminescence metal-organic cage Radiative energy transfer Chiral small molecules Bodipy Chirality

Selective separation of pyrene from mixed polycyclic aromatic hydrocarbons by a hexahedral metal-organic cage

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Chinese Chemical Letters 2024年第1期35卷 523-527页

作者： Ya-Liang Lai Juan Su Le-Xiong Wu Dong Luo Xue-Zhi Wang Xian-Chao Zhou Chuang-Wei Zhou Xiao-Ping Zhou Dan Li College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China

Polycyclic aromatic hydrocarbons(PAHs)play an important role in the industry,and the development of new materials for the selective separation of PAHs is of great *** this work,we report a hexahedral metal-organic cage with low symmetry by subcomponent *** this cage,the eight ZnII centers adopt an interestin∧∧/△△△△△△or∧∧∧∧∧∧/△△*** cage with a cavity volume of 520˚A3 can bind anthracene,phenanthrene,and pyrene to form 1:1 host-guest complexes,while the bigger triphenylene,chrysene,perylene,and coronene cannot be *** binding constant Ka of pyrene is about 1.110×10^(3)(mol/L)^(−1),which is more than an order of magnitude larger than that of anthracene and phenanthrene(111(mol/L)^(−1),277(mol/L)^(−1),respectively).X-ray structure studies reveal that the pyrene is located in the cavity and stabilized by multiple C–H…π*** separation from a mixture of PAHs,pyrene with>96.1%purity can be *** work provides a useful method for the first time for the selective separation of pyrene from PAHs mixture by utilizing a metal-organic cage as the material,making it a useful tool for purifying and separating specific compounds from complex mixtures.

关键词： Polycyclic aromatic hydrocarbons metal-organic cage Host-guest chemistry Selective separation

An iridium(Ⅲ)-palladium(Ⅱ) metal-organic cage for efficient mitochondria-targeted photodynamic therapy

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Chinese Chemical Letters 2020年第5期31卷 1183-1187页

作者： Chaojie Li Yaping Wang Yulin Lu Jing Guo Chengyi Zhu Haozhe He Xiaohui Duan Mei Pan Chengyong Su MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China School of Materials Science and Engineering and School of Chemistry Sun Yat-Sen University.Guangzhou 510275China Sun Yat-Sen Memorial Hospital Sun Yat-Sen UniversityGuangzhou 510120China

An Ir8 Pd4-heteronuclear metal-organic cage(MOC-51)was assembled from bipodal metalloligand[Ir(ppy)2(qpy)(BF4)](qpy=4,4′:2′,2″:4″,4′′′-quaterpyridine;ppy-2-phenylpridine)with Pd(Ⅱ)*** cubic barrel shaped MOC shows one-photon and two-photon excited deep-red emission,as well as large singlet oxygen quantum yields under visible light irradiation,therefore exhibiting great potentials in organelles-targeted cell imaging and photodynamic therapy(PDT).Compared with the Ir(Ⅲ)metalloligand,the Ir8 Pd4-MOC showed less dark toxicity and higher mitochondria-targeting *** localization in mitochondria overco mes the limitation of short lifetime and diffusion distance of ROS in cell,thus improved PDT effect can be obtained in low light dose usage of the *** study presents the first case of Ir-based metal-organic cages for bio-applications in successful integration of imaging diagnosis and photodynamic therapy.

关键词： metal-organic cage Photodynamic therapy Mitochondria-targeted Ir(Ⅲ)metalloligand Two-photon

In Situ Formation of Frustrated Lewis Pairs in a Zirconium metal-organic cage for Sustainable CO_(2)Chemical Fixation

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CCS Chemistry 2023年第9期5卷 1989-1998页

作者： Cheng-Xia Chen Hassan Rabaâ Haiping Wang Pui Ching Lan Yang-Yang Xiong Zhang-Wen Wei Abdullah M.Al-Enizi Ayman Nafady Shengqian Ma Department of Chemistry University of North TexasDentonTexas 76201 MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275 Department of Chemistry Ibn Tofail UniversityESCTM14000 Kenitra Department of Chemistry College of ScienceKing Saud UniversityRiyadh 11451

Sustainable CO_(2)fixation represents a facile and promising approach to constructing various valueadded ***,we contribute a robust metal-organic cage(MOC),denoted as TCPB-1,comprising a bulky Lewis acid functionalized linker,which can in situ form frustrated Lewis pairs(FLPs)upon the addition of Lewis basic substrates to efficiently drive CO_(2)***,the incorporation of Lewis acidic boron sites within TCPB-1 promotes the efficient CO_(2)conversion to potentially medicinal benzimidazole derivatives via an FLPmediated pathway,and boosts the stability/durability of the FLP *** addition,the underlying catalysis mechanism has been established by combined experimental and molecular simulation *** work not only advances FLP/MOC as a new type of highly efficient catalyst for CO_(2)chemical fixation,but also opens a new avenue to design heterogeneous FLP-based catalysts for small molecule activation and beyond.

关键词： metal-organic cage frustrated Lewis pair heterogeneous catalysis CO_(2)conversion sustainable chemistry

Effects of anions on the structural regulation of Zn‑salen‑modified metal‑organic cage

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无机化学学报 2024年第11期40卷 2203-2211页

作者： GUO Qiaojia CAI Junkai DUAN Chunying State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalianLiaoning 116024China

By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ***-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic *** to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift *** dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.

关键词： metal-organic cage Zn-salen host-guest electrostatic interaction anions structural regulation

Immobilization of metal-organic molecular cage on g-C3N4 semiconductor for enhancement of photocatalytic H2 generation

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Chinese Journal of Catalysis 2019年第8期40卷 1198-1204页

作者： Yuanpu Wang Liang Liu DongJun Wu Jing Guo Jianying Shi Junmin Liu Chengyong Su MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of Chemistryand School of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275GuangdongChina State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

A new compound based on immobilizing of Pd6(RuL3)8(BF4)28 (L=2-(pyridin-3-yl)-1H-imidazo [4,5-f][1,10]-phenanthroline) cage (MOC-16) on g-C3N4 was synthesized. Infrared spectrum and powder X-ray diffraction were used to characterize structure of hybrid MOC-16/g-C3N4, as well as UV-vis absorption spectrum and X-ray photoelectron spectroscopy were carried out to unveil photocatalytic mechanism. With the introduction of MOC-16, the absorption edge of MOC-16/g-C3N4 in UV-vis spectrum extended apparently to long-wavelength region compared with pristine g-C3N4. H2 evolution yielded with MOC-16/g-C3N4 in aqueous solution containing TEOA was much higher than that with RuL3/g-C3N4, Pd/RuL3/g-C3N4 and mixture of MOC-16 and g-C3N4, showing that the octahedral cage structure with high-efficient electron transfer and the interface interaction between MOC-16 and g-C3N4 were significant for improvement of H2 evolution.

关键词： g-C3N4 metal-organic cage Photocatalytic H2 evolution Visible light Stability