Metal–Organic Framework Thin Films Composed of Free-Standing Acicular Nanorods Exhibiting Reversible Electrochromism

Kung, Chung Wei; Wang, Timothy Chiaan; Mondloch, Joseph E.; Fairen‐Jimenez, David; Gardner, Daniel M.; Bury, Wojciech; Klingsporn, Jordan M.; Barnes, Jonathan C.; Duyne, Richard Van; Stoddart, J. Fraser; Wasielewski, Michael R.; Farha, Omar K.; Hupp, Joseph T.

doi:10.1021/cm403726v

Cited by 244 publications

(263 citation statements)

References 46 publications

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“…[1][2][3][4][5][6][7][8][9][10][11][12] The highest Brunauer-Emmett-Teller (BET) surface area of MOFs reported in literature can exceed 7000 m 2 /g, 13 which is much higher than the values of other porous materials. Due to the highsurface-area characteristic of MOF, several recent studies have utilized MOFs as electrode materials for electrochemical applications, [14][15][16][17][18][19] such as supercapacitors, fuel cells, corrosion inhibition, 20 or electrochemical energy storage and conversion. [21][22][23][24] MOFs can also hold active guest molecules, enzymes, bacteria, and nanoparticles to promote their electrochemical activity.…”

Section: Introductionmentioning

confidence: 99%

Inkjet-printed porphyrinic metal–organic framework thin films for electrocatalysis

Kung

Chang

et al. 2016

J. Mater. Chem. A

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In this study, a simple and effective direct inkjet printing method was developed to prepare porphyrinic metal-organic framework (MOF) thin films for electrocatalysis. First, crystals of a zirconium-based porphyrinic MOF (MOF-525) with crystal sizes ranging from 100 to 700 nm were synthesized by adjusting the content of benzoic acid in the solvothermal synthetic process. The synthesized crystals showed similar surface area of 2500 m 2 /g with a unique pore size of 1.85 nm. However, some structural defects was found in the smallest crystals of 100 nm due to the fast crystallization process. After suspended in dimethylformamide, the MOF crystal suspensions were inkjet printed to fabricate uniform MOF-525 thin film patterns. With the help of great precision in liquid deposition, thicknesses of the printed MOF-525 thin films can be accurately controlled by the number of printed layers. With smaller crystal size, the printed MOF thin films showed more compact stacking and better contact with the substrate. The printed MOF thin films were applied for electrocatalytic nitrite oxidation. The effects of both film thickness and crystal size on printed film morphology and electrocatalytic activity were investigated in details. The printed MOF nitrite sensor showed a great detection limit of 0.72 μM and a high sensitivity of 40.6 μA/mM-cm 2 . In summary, this study demonstrated the feasibility of the proposed printing process for electrochemically addressable MOF thin films and can be further applied for many other electrochemical applications.

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Section: Introductionmentioning

confidence: 99%

Inkjet-printed porphyrinic metal–organic framework thin films for electrocatalysis

Kung

Chang

et al. 2016

J. Mater. Chem. A

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“…polymorphs NU-901 and NU-1000, exhibit high porosity, chemical stability and conductivity, simultaneously, making these suitable for electrochemical device applications. 8,18,[38][39][40] Depending on the application, additional material requirements besides charge transport include energy transport, [41][42][43] optical response [44][45][46] and catalytic activity. 13 The catalytic activity of MOFs has been studied for a variety of reactions, including oxidation, hydrogenation and condensation reactions.…”

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confidence: 99%

Theoretical Investigation of Charge Transfer in Metal Organic Frameworks for Electrochemical Device Applications

Patwardhan

Schatz

2015

J. Phys. Chem. C

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For electrochemical device applications metal organic frameworks (MOFs) must exhibit suitable conduction properties. To this end, we have performed computational studies of intermolecular charge transfer in MOFs consisting of hexa-Zr IV nodes and tetratopic carboxylate linkers. This includes an examination of the electronic structure of linkers that are derived from tetraphenyl benzene 1, tetraphenyl pyrene 2 and tetraphenyl porphyrin 3 molecules. These results are used to determine charge transfer propensities in MOFs, within the framework of Marcus theory, including an analysis of the key parameters (charge transfer integral t, reorganization energy λ and free energy change ∆G 0 ), and evaluation of figures of merit for charge transfer based on the chemical structures of the linkers. This qualitative analysis indicates that delocalization of the HOMO/LUMO on terminal substituents increases t and decreases λ, while weaker binding to counterions decreases ∆G 0 , leading to better charge transfer propensity. Subsequently, we study hole transfer in the linker 2 containing MOFs, NU-901 and NU-1000, in detail and describe mechanisms (hopping and superexchange) that may be operative under different electrochemical conditions. Comparisons with experiment are provided whereavailable. Based on the redox and catalytic activity of nodes and linkers, we propose three possible schemes for constructing electrochemical devices for catalysis. We believe that the results of this study will lay the foundation for future experimental work on this topic.

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“…[90] Magnetic phase transitions have been investigated on a theoretical level for 2D MOFs with a range of metallic centers (Cr, Mn, Fe, Co, Ni), [91] particularly, phase transition between homogeneous ferromagnetic and spin-forming antiferromagnetic states. [92] A desired property of materials for data storage is the ability to switch magnetic domains. [91] A switch between n (electron) and p (hole) type band structures has also been observed for 2D MOFs (M 3 C 12 S 12 and M 3 C 12 O 12 , where M = Zn, Cd, Hg, Be, or Mg), due to tuneable deformation or electrostatic gating.…”

Section: Phase-change Effectmentioning

confidence: 99%

Metal–Organic Frameworks in Modern Physics: Highlights and Perspectives

et al. 2019

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Owing to the synergistic combination of a hybrid organic–inorganic nature and a chemically active porous structure, metal–organic frameworks have emerged as a new class of crystalline materials. The current trend in the chemical industry is to utilize such crystals as flexible hosting elements for applications as diverse as gas and energy storage, filtration, catalysis, and sensing. From the physical point of view, metal–organic frameworks are considered molecular crystals with hierarchical structures providing the structure‐related physical properties crucial for future applications of energy transfer, data processing and storage, high‐energy physics, and light manipulation. Here, the perspectives of metal–organic frameworks as a new family of functional materials in modern physics are discussed: from porous metals and superconductors, topological insulators, and classical and quantum memory elements, to optical superstructures, materials for particle physics, and even molecular scale mechanical metamaterials. Based on complementary properties of crystallinity, softness, organic–inorganic nature, and complex hierarchy, a description of how such artificial materials have extended their impact on applied physics to become the mainstream in material science is offered.

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Metal–Organic Framework Thin Films Composed of Free-Standing Acicular Nanorods Exhibiting Reversible Electrochromism

Cited by 244 publications

References 46 publications

Inkjet-printed porphyrinic metal–organic framework thin films for electrocatalysis

Inkjet-printed porphyrinic metal–organic framework thin films for electrocatalysis

Theoretical Investigation of Charge Transfer in Metal Organic Frameworks for Electrochemical Device Applications

Metal–Organic Frameworks in Modern Physics: Highlights and Perspectives

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