Editorial
Reticular chemistry at the atomic, molecular, and framework scales
Yue-Biao Zhang1,*, Qiaowei Li2,*, and Hexiang Deng3,*
1 ShanghaiTech University, China
2 Fudan University, China
3 Wuhan University, China
335–337
Review Articles
Let the light be a guide: Chromophore communication in metal-organic frameworks
Corey R. Martin, Preecha Kittikhunnatham, Gabrielle A. Leith, Anna A. Berseneva, Kyoung Chul Park, Andrew B. Greytak, and Natalia B. Shustova*
University of South Carolina, USA
Metal-organic framework motifs promote efficient chromophore communications and unveil the potential for a promising library of futuristic materials for advancing nanoscale photonics and portable electronics.
（點擊中文簡介）以光為指導：MOF中的發色團相互作用
338–354
Hierarchical assemblies of molecular frameworks—MOF-on-MOF epitaxial heterostructures
Ritesh Haldar and Christof Wöll*
Karlsruhe Institute of Technology (KIT), Germany
Synthetic strategies and applications of hierarchical metal-organic framework (MOF)-on-MOF epitaxial heterostructures are reviewed.
（Most downloaded）
355–368
Research Articles
Two-dimensional d–π conjugated metal−organic framework based on hexahydroxytrinaphthylene
Zheng Meng and Katherine A. Mirica*
Dartmouth College, USA
A novel d–π conjugated two-dimensional metal–organic framework Cu3(HHTN)2 using a new ligand 2,3,8,9,14,15-hexahydroxytrinaphthylene was synthesized. The resulting material has a pore aperture of 2.5 nm, tunable electrical conductivity, and temperature-dependent band gap ranging from 0.75 to 1.65 eV.
（Most downloaded）
369–375
Reticular exploration of uranium-based metal–organic frameworks with hexacarboxylate building units
Zhijie Chen1,*, Penghao Li1, Xuan Zhang1, Mohammad Rasel Mian1, Xingjie Wang1, Peng Li1, Zhichang Liu1, Michael O』Keeffe2, J. Fraser Stoddart1,3,4, and Omar K. Farha1,*
1 Northwestern University, USA
2 Arizona State University, USA
3 Tianjin University, China
4 University of New South Wales, Australia
Three uranium-based metal–organic framework (MOF) structures were synthesized from trigonal planar uranyl nodes and triptycene-based hexacarboxylate ligands with variable arm lengths.
376–380
Effects of connecting sequences of building blocks on reticular synthesis of covalent organic frameworks
De-Li Ma1,2, Cheng Qian1,2,*, Qiao-Yan Qi2, Zhong-Ri Zhong1, Guo-Fang Jiang1,*, and Xin Zhao2,*
1 Hunan University, China
2 Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, China
A model system has been established to demonstrate how connecting sequences of building blocks exert an influence on the reticular synthesis of covalent organic frameworks.
381–386
High proton conductivity in metalloring-cluster based metal-organic nanotubes
Quanjie Lin1, Yingxiang Ye1, Lizhen Liu1, Zizhu Yao1, Ziyin Li1, Lihua Wang1, Chulong Liu1,*, Zhangjing Zhang1,2,*, and Shengchang Xiang1,2,*
1 Fujian Normal University, China
2 Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, China
The inner surface of metalloring-cluster based metal-organic nanotubes (MONTs) is decorated with uncoordinated carboxylic acid groups, which can obviously enhance the proton conductivities of MONTs.
387–391
Discovery of Zr-based metal-organic polygon: Unveiling new design opportunities in reticular chemistry
Jiyeon Kim1, Dongsik Nam1, Hiroshi Kitagawa2, Dae-Woon Lim2,†,*, and Wonyoung Choe1,*
1 Ulsan National Institute of Science and Technology, Republic of Korea
2 Kyoto University, Japan
† Present address: Yonsei University, Republic of Korea
This manuscript reports a triangular metal-organic polygon as a new member of Zr-based metal-organic materials. The interplay of the geometrically frustrated ligand and secondary building unit opens up new design opportunities.
392–397
From a mononuclear FeL2 complex to a Fe4L4 molecular square: Designed assembly and spin-crossover property
Zhuo Wang1,2, Li-Peng Zhou1,2, Li-Xuan Cai1,2, Chong-Bin Tian1,2,*, and Qing-Fu Sun1,2,*
1 Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, China
2 University of Chinese Academy of Sciences, China
The spin-crossover (SCO) performance can be improved through linking the mononuclear Fe(L1)2 SCO centers into polynuclear systems Fe4(L2)4.
398–403
Large anisotropic negative thermal expansion in Cu-TDPAT metalorganic framework: A combined in situ X-ray diffraction and DRIFTS study
Mehrdad Asgari1, Ilia Kochetygov1, Hassan Abedini1,2, and Wendy L. Queen1,*
1 École Polytechnique Fédérale de Lausanne (EPFL) -Valais Wallis, Switzerland
2 Petroleum University of Technology (PUT), Iran
Cu-TDPAT (H6TDPAT = 2,4,6-tris(3,5-dicarboxylphenylamino)-1,3,5-triazine), a stable and versatile metal-organic framework with promising adsorption performance, shows unusual negative thermal expansion properties. We shed light on the mechanism of the observed negative thermal expansion (NTE) by a combination of comprehensive in situ characterization techniques.
404–410
Solid-state phase transformations toward a metal–organic framework of 7-connected Zn4O secondary building units
Jaehui Kim, Junsu Ha, Jae Hwa Lee*, and Hoi Ri Moon*
Ulsan National Institute of Science and Technology (UNIST), Republic of Korea
Multiple transformative routes toward a metal–organic framework (MOF) of 7-connected Zn4O(COO)7 secondary building units (SBUs) can be realized by controlling the SBU geometry via the addition of either basic or acidic moieties.
411–416
Applying reticular synthesis to the design of Cu-based MOFs with mechanically interlocked linkers
Alexander J. Stirk1, Benjamin H. Wilson1, Christopher A. O』Keefe1, Hazem Amarne2, Kelong Zhu3, Robert W. Schurko4, and Stephen J. Loeb1,*
1 University of Windsor, Canada
2 The University of Jordan, Jordan
3 Sun Yat-Sen University, China
4 Florida State University, USA
The concept of reticular synthesis was used to design rigid T-shaped linkers and their [2]rotaxane analogs based on a triphenylene tetracarboxylate strut akin to that used for the iconic metal-organic framework (MOF) material NOTT-101. Single-crystal X-ray diffraction was used to characterize four new Cu(II)-based MOFs prepared using these new linkers; UWCM-12 (fof), -UWCM-13 (loz) and UWCM-14 (lil) contain 「naked」 linkers and UWDM-14 (lil), analogous to UWCM-14 (lil), contains a [2]rotaxane linker. The loz topology found for β-UWCM-13 (loz) is the first example of this net. Variable-temperature, 2H solid-state NMR spectroscopy was used to probe the motion of the 24-memebered macrocycle threaded onto the rigid backbone in UWDM-14.
417–422
Controlled growth and composition of multivariate metal-organic frameworks-199 via a reaction-diffusion process
Razan Issa1, Fayrouz Abou Ibrahim1, Mazen Al-Ghoul1,2,*, and Mohamad Hmadeh1,*
1 American University of Beirut, Lebanon
2 McGill University, Canada
Multivariate MOF-199 structures are successfully synthesized via the reaction diffusion framework (RDF). The resulting functionalized and defected metal-organic frameworks (MOFs) are employed as efficient adsorbents for dye removal from water.
423–431
Dynamic properties of a flexible metal-organic framework exhibiting a unique 「picture frame」-like crystal morphology
Kenji Sumida1,2, Nao Horike1, and Shuhei Furukawa1,*
1 Kyoto University, Japan
2 University of Adelaide, Australia
A flexible metal-organic framework (MOF) of Cu2(bdc)2(bpy) is shaped into 「picture-frame」-like crystal morphology, which is correlated to the dynamic properties to vary between rigid, elastic, and shape memory modes.
432–437
Layer-by-layer assembled dual-ligand conductive MOF nano-film with modulated chemiresistive sensitivity and selectivity
Ai-Qian Wu1, Wen-Qing Wang1, Hong-Bin Zhan1, Lin-An Cao2, Xiao-Liang Ye2, Jia-Jia Zheng3, Pendyala Naresh Kumar2, Kashi Chiranjeevulu2, Wei-Hua Deng2, Guan-E Wang2, Ming-Shui Yao2,3,*, and Gang Xu2,*
1 Fuzhou University, China
2 Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, China
3 Kyoto University, Japan
We demonstrate a dual-ligand design strategy to modulate the performance of electronically conductive metal–organic framework (EC-MOF) thin film with a spray layer-by-layer assembly method. The high quality nano-film of 2,3,6,7,10,11-hexaiminotriphenylene (HITP) doped Cu-HHTP enables the precise modulation of the chemiresistive sensitivity and selectivity.
438–443
Rapid room-temperature synthesis of a porphyrinic MOF for encapsulating metal nanoparticles
Huihui He1, Luyan Li3, Yang Liu1, Meruyert Kassymova3, Dandan Li2,*, Liangliang Zhang1,*, and Hai-Long Jiang3
1 Northwestern Polytechnical University (NPU), China
2 Anhui University, China
3 University of Science and Technology of China, China
We successfully prepared a porphyrinic metal-organic framework (MOF), PCN-224-RT, as a support for encapsulating metal nanoparticles via a directly stirring method at room temperature. The rapid and simple method in this work is favorable in reference to traditional solvothermal methods.
444–449
Nickel phosphonate MOF as efficient water splitting photocatalyst
Pablo Salcedo-Abraira1,2, Sérgio M. F. Vilela1, Artem A. Babaryk1, María Cabrero-Antonino3, Pedro Gregorio1, Fabrice Salles4, Sergio Navalón3, Hermenegildo García3,*, and Patricia Horcajada1,*
1 Advanced Porous Materials Unit (APMU), Spain
2 Universidad Complutense de Madrid, Spain
3 Universitat Politècnica de València, Spain
4 Université Montpellier, France
A novel robust microporous two-dimensional (2D) Ni-phosphonate metal-organic framework (MOF) has been prepared, exhibiting without co-catalyst stable photocatalytic activity in hydrogen evolution and overall water splitting.
450–457
Heterogeneous catalysts with programmable topologies generated by reticulation of organocatalysts into metal-organic frameworks: The case of squaramide
Anna Broto-Ribas1, Claudia Vignatti1, Alicia Jimenez-Almarza2, Javier Luis-Barrera2, Zahra Dolatkhah2, Felipe Gándara3, Inhar Imaz1,*, Rubén Mas-Ballesté2,4,*, José Alemán2,4,*, and Daniel Maspoch1,5,*
1 CSIC and The Barcelona Institute of Science and Technology, Spain
2 Universidad Autonoma de Madrid, Spain
3 Consejo Superior de Investigaciones Cientificas (CSIC), Spain
4 Campus Universidad Autonoma de Madrid, Spain
5 Institucio Catalana de Recerca i Estudis Avancats (ICREA), Spain
A series of metal-organic framework (MOF)-based catalysts with programmable topologies are generated by incorporating squaramide organocatalysts, using reticular chemistry and exploiting MOF-structural data from Cambridge Structural Database.
458–465
Chiral metal–organic frameworks with tunable catalytic selectivity in asymmetric transfer hydrogenation reactions
Xu Chen1, Zhiwei Qiao2, Bang Hou1, Hong Jiang1, Wei Gong1, Jinqiao Dong1, Hai-Yang Li3, Yong Cui1, and Yan Liu1,*
1 Shanghai Jiao Tong University, China
2 Guangzhou University, China
3 Zhengzhou University, China
We have demonstrated that the enantioselectivity of metal–organic framework (MOF) catalysts in asymmetric transfer hydrogenation of heteroaromatic imines could be rationally tuned by changing the electronegativities of metal ions and modifying the steric hindrance of ligand structures of MOFs.
466–472
Metal-organic layers as reusable solid fluorination reagents and heterogeneous catalysts for aromatic fluorination
Wenjie Shi1,2, Lingzhen Zeng1, Lingyun Cao1, Ying Huang1, Cheng Wang1,*, and Wenbin Lin2
1 Xiamen University, China
2 University of Chicago, USA
A Pd-functionalized two-dimensional metal-organic layer (MOL) was developed as a heterogeneous catalyst and a reusable solid reagent to fluorinate a broad scope of aromatic compounds. The MOL stabilized a highly reactive N-fluoroxy-phenanthrolinium coordinated on Pd as the active center in the solid reagent, highlighting new opportunities in fluorination chemistry with MOLs.
473–478
Direct aerobic oxidation of monoalcohol and diols to acetals using tandem Ru@MOF catalysts
Songwei Zhang1,3, Jerry Pui Ho Li1,5, Jingpeng Zhao2, Dan Wu2, Biao Yuan1, Willinton Yesid Hernández2, Wen-Juan Zhou2, Tao He1,4, Yi Yu1, Yong Yang1,*, Vitaly Ordomsky2,*, and Tao Li1,*
1 ShanghaiTech University, China
2 Eco-Efficient Products and Processes Laboratory (E2P2L), China
3 University of Chinese Academy of Sciences, China
4 Shanghai Advanced Research Institute, Chinese Academy of Sciences, China
5 Queen’s University Belfast, UK
The existing methods usually rely on a two-step process in which alcohols are first oxidized to aldehydes over metal catalysts (Ru, Pt, Pd) and then acetalized using acids. Hereby we report a Ru@MOF tandem catalyst containing ultra-fine Ru nanoparticles (< 2 nm) for direct alcohol to acetal conversion of monoalcohols and diols with no formation of carboxylic acids.
479–485
Single-atom Pd catalyst anchored on Zr-based metal-organic polyhedra for Suzuki-Miyaura cross coupling reactions in aqueous media
Seongsoo Kim1, Seohyeon Jee2, Kyung Min Choi2,*, and Dong-Sik Shin2,*
1 Kangwon National University, Republic of Korea
2 Sookmyung Women’s University, Republic of Korea
The discrete cages of metal-organic polyhedra anchoring single Pd atom successfully catalyse a Suzuki-Miyaura cross coupling reaction with various substrates in aqueous media.
486–492
Highly efficient multi-metal catalysts for carbon dioxide reduction prepared from atomically sequenced metal organic frameworks
Celia Castillo-Blas1,†, Consuelo Álvarez-Galván2,*, Inés Puente-Orench3,4, Alba García-Sánchez5, Freddy E. Oropeza5, Enrique Gutiérrez-Puebla1, Ángeles Monge1,*, Víctor A. de la Peña-O』Shea5,*, and Felipe Gándara1,*
1 Materials Science Institute of Madrid (CSIC), Spain
2 Instituto de Catálisis y Petroleoquímica (CSIC), Spain
3 Instituto de Ciencia de Materiales de Aragón, Spain
4 Institut Laue Langevin, France
5 Photoactivated Processes Unit IMDEA Energy Institute, Spain
† Present address: University Autonomous of Madrid, Spain
Precision at the atomic level exerted in metal-organic frameworks (MOFs) allows control on the formation of complex nanomaterials with enhanced reactivity: Supported metal nanoparticles are formed from MOF derived multi-metal oxides, and are efficient catalyst for the reduction of carbon dioxide in the reverse water-gas shift reaction.
493–500
Oxygen vacancy engineering of calcium cobaltate: A nitrogen fixation electrocatalyst at ambient condition in neutral electrolyte
Xinyu Chen, Ke Li, Xiaoxuan Yang, Jiaqi Lv, Sai Sun, Siqi Li, Dongming Cheng, Bo Li, Yang-Guang Li, and Hong-Ying Zang*
Northeast Normal University, China
Herein, a calcium metalate catalyst CaCoOx nanoplates with oxygen vacancies was synthesized and used as an electrocatalyst for nitrogen reduction reaction (NRR) for the first time, whose morphology can be controlled by the calcination temperature and the heating rate. Under the optimal conditions, the CaCoOx catalyst achieved the yield of nitrogen conversion to ammonia of 16.25 μg·h−1·mgcat.−1 and showed good stability even after 12 times recyclability.
501–506
A microporous aluminum-based metal-organic framework for high methane, hydrogen, and carbon dioxide storage
Bin Wang1,2, Xin Zhang2, Hongliang Huang4, Zhangjing Zhang1, Taner Yildirim3, Wei Zhou3, Shengchang Xiang1,*, and Banglin Chen2,*
1 Fujian Normal University, China
2 University of Texas at San Antonio, USA
3 National Institute of Standards and Technology, USA
4 Tianjin Polytechnic University, China
In this work, we explored the methane, hydrogen, and carbon dioxide storage capacities of a stable microporous aluminum-based metal-organic framework with large surface area and pore volume.
507–511
A robust soc-MOF platform exhibiting high gravimetric uptake and volumetric deliverable capacity for on-board methane storage
Gaurav Verma1, Sanjay Kumar1,†,*, Harsh Vardhan1, Junyu Ren1, Zheng Niu1, Tony Pham1,‡, Lukasz Wojtas1, Sydney Butikofer1,⊥, Jose C Echeverria Garcia1, Yu-Sheng Chen2, Brian Space1, and Shengqian Ma1,*
1 University of South Florida, USA
2 The University of Chicago, USA
† Present address: Multani Mal Modi College, India
‡ Present address: The University of Tampa, USA
⊥ Present address: University of Illinois at Urbana-Champaign, USA
An iron-based square-octahedron (soc) topology metal-organic framework (soc-MOF) shows high gravimetric uptake and volumetric deliverable capacity for methane storage at 65 bar and room temperature.
512–517
Highly effective H2/D2 separation in a stable Cu-based metalorganic framework
Yanan Si1,3, Xiang He2,*, Jie Jiang2, Zhiming Duan2, Wenjing Wang1, and Daqiang Yuan1,*
1 Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, China
2 Shanghai University, China
3 University of the Chinese Academy of Sciences, China
Efficient hydrogen isotope separation is achieved by using the dynamic low-temperature breakthrough device, in which a mixed gas of H2/D2/Ne (10/10/80, vol.%) flowed over the packed column of activated FJI-Y11 with a total flow of 10 mL/min at 77 K and 1 bar.
518–525
Separation of hexane isomers by introducing 「triangular-like and quadrilateral-like channels」 in a bcu-type metal-organic framework
Dongmei Wang1,2, Xinglong Dong3, Yu Han3,*, and Yunling Liu1,*
1 Jilin University, China
2 Zhejiang Normal University, China
3 King Abdullah University of Science and Technology, Kingdom of Saudi Arabia
A novel bcu-type metal-organic framework (MOF) Zn9(tba)9(dabco)3 (H2tba = 4-(1H-tetrazol-5-yl)-benzoic acid; dabco = 1,4-diazabicyclo[2.2.2]octane) with triangular-like and quadrilateral-like channels was designed and assembled based on reticular chemistry strategy. Resulting from the synergetic contributory of sieving effect and diffusion, Zn9(tba)9(dabco)3 exhibits highly effective separation ability for hexane isomers.
526–531
Efficient hexane isomers separation in isoreticular bipyrazolate metal-organic frameworks: The role of pore functionalization
Rebecca Vismara1,†, Corrado Di Nicola2, Rodrigo Gil-San Millán3, Kostiantyn V. Domasevich4, Claudio Pettinari2,5, Jorge A. R. Navarro3,*, and Simona Galli1,6,*
1 Universita dell』Insubria, Italy
2 University of Camerino, Italy
3 Universidad de Granada, Spain
4 Taras Shevchenko National University of Kyiv, Ukraine
5 Istituto di Chimica dei Composti Organometallici (ICCOM-CNR), Italy
6 Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali, Italy
† Present address: University of Liverpool, UK
Pore functionalization in a series of robust isoreticular zinc-bipyrazolate frameworks possessing square one-dimensional channels gives rise to selective hexane isomers adsorption interactions leading to efficient gas separation, as proven by experimental and computational studies.
532–540
Remarkable separation of C5 olefins in anion-pillared hybrid porous materials
Ying Yu1, Lifeng Yang1,2, Bin Tan3, Jianbo Hu1,2, Qingju Wang1, Xili Cui1,2,*, and Huabin Xing1,2
1 Zhejiang University, China
2 Institute of Zhejiang University-Quzhou, China
3 CHN Energy, China
Anion-pillared hybrid porous materials with well-distributed anion-based electrostatic environment and responsive flexible skeleton exhibit remarkable separation and regeneration performance for C5 olefin mixtures of trans-2-pentene, 1-pentene and isoprene.
541–545
A chemically stable nanoporous coordination polymer with fixed and free Cu2+ ions for boosted C2H2/CO2 separation
Si Chen1, Nibedita Behera1, Chao Yang1, Qiubing Dong1, Baishu Zheng2, Yingying Li1, Qi Tang1, Zhaoxu Wang2,*, Yanqing Wang3,*, and Jingui Duan1,*
1 Nanjing Tech University, China
2 Hunan University of Science and Technology, China
3 Yancheng Teachers University, China
A new chemically stable nanoporous coordination polymer adsorbent with fixed and free Cu ions was prepared through post-synthetic approach, which shows excellent C2H2/CO2 separation, along with enhanced C2H2 capacity.
546–553
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