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Photochemical cycloaddition and temperature-dependent breathing in pillared-layer metal–organic frameworks

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Science Bulletin 2019年第24期64卷 1881-1889页

作者： Qingqing Pang Binbin Tu Lingyi Yang Qiaowei Li Department of chemistry Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) and Shanghai Key Laboratory of Molecular Catalysis and InnovativeMaterials Fudan University

Single crystallinity of metal–organic frameworks(MOFs) enables the studies of their flexible behaviors with atomic precision. Here, we investigated the structural transformations triggered by photochemical cycloaddition and with temperature-dependent breathing in a series of pillared-layer MOF structures using a variety of pyrazolecarboxylate linkers for the layers and bipyridyl linkers as the pillars. The ethylenic double bonds from the pillars in close proximity undergo quantitative and seteroselective photochemical [2 + 2] cycloaddition upon UV irradiation, transforming the MOFs into structures with cyclobutane-based pillars. Furthermore, reversible breathing of the new pillared-layer MOF was evidenced by the 10.8% unit cell parameter change along c axis upon temperature change between 298 and 173 K. As revealed by single crystal X-ray diffraction, this transformation originates from the relative flattening of the wavy layers upon cooling. These two different types of characteristic structural transformations responding to inherent reactions and external stimuli happen at single crystalline state, providing a well-defined robust system with controlled flexibility.

关键词： Pillared-layer MOF Photochemical cycloaddition Structural transformation Breathing MOF reticular chemistry

Design,synthesis and applications of functional zirconium-based metal-organic frameworks

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Science China chemistry 2023年第12期66卷 3383-3397页

作者： Le Shi Zhenning Yang Fanrui Sha Zhijie Chen Stoddart Institute of Molecular Science Department of ChemistryZhejiang UniversityHangzhou 310058China Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation CenterZhejiang UniversityHangzhou 311215China Department of chemistry and International Institute for Nanotechnology Northwestern UniversityEvanstonIllinois 60208United States

Zirconium-based metal-organic frameworks(Zr-MOFs)have been explored for applications including but not limited to water adsorption,gas storage and separation,heterogeneous catalysis,and chemical ***-MOFs serve as a major class of functional MOFs thanks to their high thermal,chemical and hydrolytic stability,large surface area,and tunable structures with the versatile *** this work,we highlight the design and synthesis of zirconium-based MOFs as well as their ***,we demonstrate how reticular chemistry can direct the rational design and synthesis of functional ZrMOFs and describe their structure–property *** addition,we feature synthetic strategies,including isoreticular expansion,linker functionalization,node functionalization,and defect engineering,as toolkits to construct tailored material for specific applications.

关键词： metal-organic frameworks Zr-MOFs reticular chemistry structure–property relationship

Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers

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Nano Research 2021年第2期14卷 417-422页

作者： Alexander J.Stirk Benjamin H.Wilson Christopher A.O’Keefe Hazem Amame Kelong Zhu Robert W.Schurko Stephen J.Loeb Department of chemistry and Biochemistry University of WindsorWindsorOntarioN9B 3B4Canada Department of chemistry The University of JordanAmman11942Jordan School of chemistry Sun Yat-Sen UniversityGuangzhou 510275China Department of chemistry and Biochemistry Florida State UniversityTallahasseeFlorida 32306-4390USA

The concept of“robust dynamics”describes the incorporation of mechanically interlocked molecules(MIMs)into metal-organic framework(MOF)materials such that large amplitude motions(e.g.,rotation or translation of a macrocycle)can occur inside the free volume pore of the *** aid in the preparation of such materials,reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF *** linkers were synthesized that have a T-shape,based on a triphenylene tetra-carboxylate strut,and their incorporation into Cu(II)-based MOFs was *** single-crystal structures of three new MOFs,UWCM-12(fof),β-UWCM-13(loz),UWCM-14(lil),with naked T-shaped linkers were determined;β-UWCM-13 is the first reported example of the loz topology.A fourth MOF,UWDM-14(lil)is analogous to UWCM-14(lil)but contains a[2]rotaxane ***-temperature,^(2)H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton.

关键词： reticular chemistry metal-organic frameworks mechanically interlocked molecules rotaxane

Topology control of three-dimensional covalent organic frameworks by adjusting steric hindrance effect

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Science China chemistry 2022年第11期65卷 2177-2181页

作者： Yang Xie Meng Liu Honglin Du Bo Gui Junliang Sun Cheng Wang Sauvage Center for Molecular Sciences College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China College of chemistry and Molecular Engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing100871China

Since the intrinsic topological network determines their pore characteristics and functional applications, it is important to construct 3D COFs with target topology from predesigned functional building blocks. However, when starting from precursors with same connectivity but different bulky groups, the structure and topology of 3D COFs may change, which will greatly increase the complexity of the crystal structure determination. Therefore, it is essential to understand how to control the steric hindrance effects and synthesize 3D COFs with target topology. Herein, we report the topology control of 3D COFs by adjusting steric hindrance effects of functional building blocks. Starting from a quadrilateral building block with sterically hindered phenyl groups, we have been able to achieve the target pts topology instead of the unprecedented ljh network that we reported recently by elongating the tetrahedral building block. This result clearly shows that it is promising to precisely control the topology of 3D COFs by judiciously selecting building blocks with steric hindrance and suitable dimensions.

关键词： COF 3D reticular chemistry topology control steric hindrance effect

Atomically precise metal chalcogenide supertetrahedral clusters:frameworks to molecules,and structure to function

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National Science Review 2022年第1期9卷 128-143页

作者： Jiaxu Zhang Pingyun Feng Xianhui Bu Tao Wu College of chemistry Chemical Engineering and Material Science Soochow University Department of chemistry University of California College of chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University Department of chemistry and Biochemistry California State University

Metal chalcogenide supertetrahedral clusters(MCSCs) are of significance for developing crystalline porous framework materials and atomically precise cluster *** research interest focused on the synthetic and structural chemistry of MCSC-based porous semiconductor materials with different cluster sizes/compositions and their applications in adsorption-based separation and *** recently,focus has shifted to the cluster chemistry of MCSCs to establish atomically precise structure-composition-property relationships,which are critical for regulating the properties and expanding the applications of ***,MCSCs are similar to Ⅱ-Ⅵ or Ⅰ-Ⅲ-Ⅵ semiconductor nanocrystals(also called quantum dots,QDs) but avoid their inherent size polydispersity and structural ***,discrete MCSCs,especially those that are solution-processable,could provide models for understanding various issues that cannot be easily clarified using *** review covers three decades of efforts on MCSCs,including advancements in MCSC-based open frameworks(reticular chemistry),the precise structure-property relationships of MCSCs(cluster chemistry),and the functionalization and applications of MCSC-based micro *** outlook on remaining problems to be solved and future trends is also presented.

关键词： metal chalcogenide nanocluster open framework semiconductor reticular chemistry atomically precise nanochemistry

A robust soc-MOF platform exhibiting high gravimetric uptake and volumetric deliverable capacity for on-board methane storage

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Nano Research 2021年第2期14卷 512-517页

作者： Gaurav Verma Sanjay Kumar Harsh Vardhan Junyu Ren Zheng Niu Tony Pham Lukasz Wojtas Sydney Butikofer Jose C Echeverria Garcia Yu-Sheng Chen Brian Space and Shengqian Ma Department of chemistry University of South Florida4202 E.Fowler Ave.TampaFL 33637USA ChemMatCARS Center for Advanced Radiation SourcesThe University of Chicago9700 South Cass AvenueArgonneIL 60439USA Department of chemistry Multani Mai Modi CollegePatiala 147001India Department of chemistry Biochemistryand PhysicsThe University of Tampa401 W.Kennedy Blvd.TampaFL 33606-1490USA Department of Chemical and Biomolecular Engineering University of Illinois at Urbana-ChampaignChampaignIL 61801USA

Emerging as an outperformed class of metal-organic frameworks(MOFs),square-octahedron(soc)topology MOFs(soc-MOFs)feature superior properties of high porosity,large gas storage capacity,and excellent thermal/chemical *** report here an iron based soc-MOF,denoted as Fe-pbpta(H4pbpta=4,4',4'',4'''-(1,4-phenylenbis(pyridine-4,2-6-triyl))-tetrabenzoic acid)possessing a very high Brunauer,Emmett and Teller(BET)surface area of 4,937 m2/g and a large pore volume of 2.15 cm3/*** MOF demonstrates by far the highest gravimetric uptake of 369 cm3(STP)/g under the DOE operational storage conditions(35 bar and 298 K)and a high volumetric deliverable capacity of 192 cc/cc at 298 K and 65 ***,Fe-pbpta exhibits high thermal and aqueous stability making it a promising candidate for on-board methane storage.

关键词： metal-organic framework(MOF) reticular chemistry methane storage aqueous stability high gravimetric and volumetric uptake

Effects of connecting sequences of building blocks on reticular synthesis of covalent organic frameworks

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Nano Research 2021年第2期14卷 381-386页

作者： De-Li Ma Cheng Qian Qiao-Yan Qi Zhong-Ri Zhong Guo-Fang Jiang Xin Zhao State Key Lab of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan Universityf Changsha 410082China Key Laboratory of Synthetic and Self-Assembly chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of Sciences345 Lingling RoadShanghai 200032China

The principle of reticular chemistry has been widely used to guide the design of crystalline porous materials such as metal organic frameworks(MOFs)and covalent organic frameworks(COFs).While in the early strategies only the symmetries of the building blocks were considered for reticular synthesis of COFs,recently a few researches on COFs with hierarchical porosities indicate that connecting sequence of building blocks also plays a crucial role in determining crystalline structures of ***,this important phenomenon has not been systematically investigated *** this article,a model system has been established to demonstrate how different connecting sequences of two C_(2v)-symmetric building blocks lead to the formation of four two-dimensional(2D)COFs with distinct framework *** verify this concept,target synthesis was conducted to produce three COFs,whose structures were confirmed by powder X-ray diffraction and pore size distribution analysis.

关键词： reticular chemistry covalent organic framework connecting sequence building block

Highly selective adsorption of light hydrocarbons in a HKUST-like MOF constructed from spirobifluorene-based octacarboxylate ligand by a substitution strategy

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Nano Research 2023年第7期16卷 10652-10659页

作者： Xinli Shi Yucong Zu Xilin Li Tongyi Zhao Hao Ren Fuxing Sun State Key Laboratory of Inorganic Synthesis and Preparative chemistry Jilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)with HKUST-like tbo structures have been paid specific attention for gas sorption and separation because of their specific pore *** to the geometric similarity of spirobifluorene and[Cu_(2)(O_(2)CR)_(4)]paddlewheel secondary building units(Cu_(2)SBUs)in HKUST-1,we attempted to rationally construct a HKUST-like MOF by a substitution *** a judiciously designed octatopic carboxylate ligand,a copper-organic framework,JUC-220,was *** crystals of JUC-220 exhibited characteristic features in cubic with disorder,possibly due to the disorder substitution and high symmetry of tbo *** related HKUST-like structure models were *** to the suitable pore size and specific pore shapes,the adsorption selectivities of JUC-220 for C_(3)H_(8)/CH_(4)(5/85)and C_(2)H_(6)/CH_(4)(10/85)gas mixtures were as high as 736 and 46 respectively at 298 K and 1 ***,JUC-220 exhibited excellent trace adsorption performance of C_(3)H_(8)and C_(2)H_(6)as well as reverse adsorption behavior of C_(2)H_(6)/C_(2)H_(4).Thus,JUC-220 serves as an example of HKUST-like MOF with disorder for light hydrocarbons separation and the implementation of substitution which can be used to explore more porous MOFs.

关键词： HKUST-like metal-organic frameworks(MOFs) reticular chemistry disorder substitution trace adsorption light hydrocarbons separation

Heterogeneous catalysts with programmable topologies generated by reticulation of organocatalysts into metal-organic frameworks:The case of squaramide

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Nano Research 2021年第2期14卷 458-465页

作者： Anna Broto-Ribas Claudia Vignatti Alicia Jimenez-Almarza Javier Luis-Barrera Zahra Dolatkhah Felipe Gandara Inhar Imaz Ruben Mas-Balleste Jose Aleman Daniel Maspoch Catalan Institute of Nanoscience and Nanotechnology(ICN2) CSIC and The Barcelona Institute of Science and Technology08193 BarcelonaSpain Inorganic chemistry Department Modulo 7Universidad Autonoma de Madrid28049 MadridSpain Organic chemistry Department Modulo 1Universidad Autonoma de Madrid28049 MadridSpain Materials Science Factory Instituto de Ciencia de Materiales de Madrid(ICMM)Consejo Superior de Investigaciones Cientificas(CSIC)Calle Sor Juana Ines de la Cruz328049 MadridSpain Institute for Advanced Research in Chemical Sciences(IAdChem) Campus Universidad Autonoma de Madrid28049 MadridSpain Institucio Catalana de Recerca i Estudis Avangats(ICREA) 08100 BarcelonaSpain

A well-established strategy to synthesize heterogeneous,metal-organic framework(MOF)catalysts that exhibit nanoconfinement effects,and specific pores with highly-localized catalytic sites,is to use organic linkers containing organocatalytic ***,we report that by combining this linker approach with reticular chemistry,and exploiting three-dimensioanl(3D)MOF-structural data from the Cambridge Structural Database,we have designed four heterogeneous MOF-based catalysts for standard organic *** programmable MOFs are isoreticular versions of pcu IRMOF-16,feu UiO-68 and pillared-pcu SNU-8X,the three most common topologies of MOFs built from the organic linker p.p'-terphenyldicarboxylic acid(tpdc).To synthesize the four squaramide-based MOFs,we designed and synthesized a linker,4,4’-((3,4-dioxocyclobut-1-ene-1,2-diyl)bis(azanedyil))dibenzoic acid(Sq_tpdc),which is identical in directionality and length to tpdc but which contains organocatalytic squaramide *** were chosen because their immobilization into a framework enhances its reactivity and stability while avoiding any self-quenching ***,the four MOFs share the same organocatalytic squaramide moiety,but confine it within distinct pore *** then evaluated these MOFs as heterogeneous H-bonding catalysts in organic transformations:a Friedel-Crafts alkylation and an epoxide *** of them exhibited good performance in both reactions but all showed distinct catalytic profiles that reflect their structural differences.

关键词： reticular chemistry metal-organic frameworks H-bond catalysis squaramide Friedel-Cratts epoxide ring-opening