Zeitschriftenartikel: „Conductive 2D-MOFs“

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Li, Ruofan, Xiaoli Yan und Long Chen. „2D Conductive Metal–Organic Frameworks for Electrochemical Energy Application“. Organic Materials 06, Nr. 02 (Mai 2024): 45–65. http://dx.doi.org/10.1055/s-0044-1786500.

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Two-dimensional conductive metal–organic frameworks (2D c-MOFs) have attracted research attention, benefitting from their unique properties such as superior electronic conductivity, designable topologies, and well-defined catalytic/redox-active sites. These advantages enable 2D c-MOFs as promising candidates in electrochemical energy applications, including supercapacitors, batteries and electrocatalysts. This mini-review mainly highlights recent advancements of 2D c-MOFs in the utilization for electrochemical energy storage, as well as the forward-looking perspective on the future prospects of 2D c-MOFs in the field of electrochemical energy.Table of content:1 Introduction2 Design Principles of 2D c-MOFs3 Synthesis of 2D c-MOFs4 2D c-MOFs for Electrochemical Energy Storage4.1 Supercapacitors4.2 Metallic Batteries4.2.1 Lithium-Ion Batteries4.2.2 Sodium-Ion Batteries4.2.3 Zinc-Ion Batteries4.2.4 Sodium–Iodine Batteries4.2.5 Lithium–Sulfur Batteries4.2.6 Potassium-Ion Batteries5 2D c-MOFs for Electrochemical Energy Conversion6 Conclusions and Outlook

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Guo, Yuxuan, Kuaibing Wang, Ye Hong, Hua Wu und Qichun Zhang. „Recent progress on pristine two-dimensional metal–organic frameworks as active components in supercapacitors“. Dalton Transactions 50, Nr. 33 (2021): 11331–46. http://dx.doi.org/10.1039/d1dt01729b.

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Recent progress on 2D conductive MOFs and 2D layered MOFs containing pillar-layered MOFs and 2D nanosheets as electrode materials in SCs is reviewed, including synthetic design strategies, electrochemical performances, and working mechanisms.

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Wang, Kuai-Bing, Rong Bi, Zi-Kai Wang, Yang Chu und Hua Wu. „Metal–organic frameworks with different spatial dimensions for supercapacitors“. New Journal of Chemistry 44, Nr. 8 (2020): 3147–67. http://dx.doi.org/10.1039/c9nj05198h.

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Recent progress in MOF materials for SCs with different spatial dimensions, such as 2D MOFs, including conductive MOFs and nanosheets, and 3D MOFs, categorized as single metallic and multiple metallic MOFs, are reviewed.

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Lu, Shun, Hongxing Jia, Matthew Hummel, Yanan Wu, Keliang Wang, Xueqiang Qi und Zhengrong Gu. „Two-dimensional conductive phthalocyanine-based metal–organic frameworks for electrochemical nitrite sensing“. RSC Advances 11, Nr. 8 (2021): 4472–77. http://dx.doi.org/10.1039/d0ra10522h.

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Jia, Hongxing, Yuchuan Yao, Jiangtao Zhao, Yuyue Gao, Zhenlin Luo und Pingwu Du. „A novel two-dimensional nickel phthalocyanine-based metal–organic framework for highly efficient water oxidation catalysis“. Journal of Materials Chemistry A 6, Nr. 3 (2018): 1188–95. http://dx.doi.org/10.1039/c7ta07978h.

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For the first time, we report herein bottom-up fabrication of a conductive nickel phthalocyanine-based 2D MOF and use it as a highly active electrocatalyst for OER (overpotential < 250 mV) without further pyrolysis or adding conductive materials, which can facilitate the development of 2D MOFs for energy applications.

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Ko, Michael, Lukasz Mendecki und Katherine A. Mirica. „Conductive two-dimensional metal–organic frameworks as multifunctional materials“. Chemical Communications 54, Nr. 57 (2018): 7873–91. http://dx.doi.org/10.1039/c8cc02871k.

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Two-dimensional (2D) conductive metal–organic frameworks (MOFs) have emerged as a unique class of multifunctional materials with broad applicability in electronics, chemical sensing, gas capture, catalysis, and energy conversion and storage.

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Jia, Hongxing, Shun Lu und Zhengrong Gu. „(Digital Presentation) Conductive Phthalocyanine-Based Metal-Organic Frameworks for Flexible Energy Storage Application“. ECS Meeting Abstracts MA2023-01, Nr. 15 (28.08.2023): 1445. http://dx.doi.org/10.1149/ma2023-01151445mtgabs.

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Recently, two-dimensional conductive MOFs (2D c-MOFs) with improved intrinsic electrical conductivity have been synthesized and employed as electrocatalysts, gas sensors, supercapacitors, and so on. In previous literature, 2D c-MOFs were usually synthesized initially as the powder/film through solvothermal approach, after which a transfer and/or reshaping process is necessary for the electrode fabrication [1-3]. In most cases, the electrodes of 2D c-MOFs were prepared with conductive additives and binders through the slurry coating method [2]. In doing so, their superior intrinsic conductivity over traditional MOFs was obscured. Moreover, the use of additives might reduce the effective surface area and negatively affect long-term cycling performance. To avoid the use of additives, 2D c-MOFs could be pressed into self-supported pellets. Unfortunately, due to dense packing under high pressure, many MOF particles inside pellets are not able to capture ions, leading to the decrease in capacitance. Until now, restrained by flawed electrode fabrication approaches, the potential of 2D c-MOFs in supercapacitors was still far from fully exploited. The electrochemical deposition technique is a promising approach to fabricating 2D c-MOFs as electrodes, with significant advantages over above methods [3]. On the one hand, electrochemical deposition allows in situ growth of 2D c-MOFs on substrates, thus reducing the cost and simplifying the process. On the other hand, binders, conductive additives, and compacting processes are no longer necessary, which will help improve the capacitor performance [4]. Moreover, the electrochemical deposition process could be conducted at mild conditions and all parameters could be precisely controlled, which makes it a mild, facile method with good reproducibility. To date, there is still no study to prepare 2D c-MOFs through direct electrochemical deposition. In 2018, we reported the first synthesis of phthalocyanine-based 2D c-MOF nanosheets (NiPc-MOF) and its outstanding performance toward water oxidation [3]. Owing to the high electrical conductivity (~0.2 S cm-1) and large surface area (~593 m2 g-1), NiPc-MOF is also considered as a promising electrode material for supercapacitors. In this work, NiPc-MOF was grown in situ on nickel foam (NF) via the anodic electrodeposition (AED) approach (abbreviated as NiPc-MOFAED or NiPc-MOFAED@NF, Fig. 1a-d). As far as we know, the AED approach has never been used for the synthesis of 2D c-MOFs. Remarkably, the as-prepared NiPc-MOFAED@NF can be directly utilized as electrodes for flexible supercapacitors, which has also been well explored in this work. The simplified electrode fabrication process, that does not involve binders and conductive additives, would significantly reduce the cost and will have enormous potential for the applications of NiPc-MOF in energy storage. The outstanding performance of the NiPc-MOFAED@NF supercapacitor (Fig. 1e-f), including high specific areal capacitances (11.5 mF cm-2 in aqueous electrolyte and 22.1 mF cm-2 in organic electrolyte), preeminent areal power density (1.35 mW cm-2 at 1 mA cm-2, organic system) and energy density (22.4 μWh cm-1 at 0.1 mA cm-2, organic system), robust cycling stability as well as prominent mechanical ﬂexibility, were further disclosed by electrochemical measurements. This present work not only reported an advanced phthalocyanine-based MOF material for a high-performance supercapacitor, but also opens up a novel avenue for the in situ growth of the 2D c-MOF. [Figure insert] Figure 1. (a) Schematic illustration of NiPc-NiN4-MOF; (b) XRD pattern, (c) High-resolution TEM image, and (d) EDX mappings of NiPc-NiN4-MOF. NiPc-MOFAED@NF-based supercapacitor in aqueous system (PVA/LiClO4). (a) GCD curves at various current densities of 0.04-0.4 mA cm−2. (b) CV curves of supercapacitor at bending angles of 0°, 30°, 60°, and 90°. Scan rate: 20 mV s−1. (c) Photograph of a red LED powered by the three series-connected supercapacitors; NiPc-MOFAED@NF-based supercapacitor in organic system (TEABF4/Acetonitrile). (d) GCD curves at various current densities of 0.1-1 mA cm−2. (e) CV curves of supercapacitor at bending angles of 0°, 30°, 60°, and 90°. Scan rate: 100 mV s−1. (f) Photograph of a green LED powered by one supercapacitor. (Ref: Journal of Power Sources, 2022, 526: 231163) Copyright 2022 Elsevier. Reference: [1] Jia, Hongxing, et al. "In situ anodic electrodeposition of two-dimensional conductive metal-organic framework@nickel foam for high-performance flexible supercapacitor." Journal of Power Sources 526 (2022): 231163. [2] Lu, Shun, et al. "Two-dimensional conductive phthalocyanine-based metal–organic frameworks for electrochemical nitrite sensing." RSC Advances 11.8 (2021): 4472-4477. [3] Jia, Hongxing, et al. "A novel two-dimensional nickel phthalocyanine-based metal–organic framework for highly efficient water oxidation catalysis." Journal of Materials Chemistry A 6.3 (2018): 1188-1195. [4] Yan, Caihong, et al. "Hydrothermal synthesis of vanadium doped nickel sulfide nanoflower for high-performance supercapacitor." Journal of Alloys and Compounds 928 (2022): 167189. Figure 1

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Le, Khoa N., Jenna L. Mancuso und Christopher H. Hendon. „Electronic Challenges of Retrofitting 2D Electrically Conductive MOFs to Form 3D Conductive Lattices“. ACS Applied Electronic Materials 3, Nr. 5 (29.04.2021): 2017–23. http://dx.doi.org/10.1021/acsaelm.0c01135.

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Xie, Sijie, und Jan Fransaer. „Cathodic Deposition of Conductive MOF Films: Mechanism and Applications“. ECS Meeting Abstracts MA2023-02, Nr. 21 (22.12.2023): 1294. http://dx.doi.org/10.1149/ma2023-02211294mtgabs.

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Conductive metal-organic frameworks (MOFs) are porous yet electric conductive, promising for many applications such as electronics, electrocatalysts, and energy storage. However, traditional solvothermal and microwave synthesis methods usually lead to MOF powders that cannot be used directly, i.e., additional processes like adding binders, casting, and thermal treatments are required for their applications. Therefore, shaping conductive MOFs into 2D thin films is attracting attention from researchers. Here we report a cathodic deposition for the one-step fabrication of conductive MOF films, which features a fast and convenient deposition process. In this method, the deposition precursor contains metal salts and organic linkers (no supporting electrolyte is needed). When an external negative bias is applied on the conductive working electrode (WE), the linkers can be deprotonated on its surface. A conductive MOF film can thus be deposited on the WE by coordinating the deprotonated linkers and metal nodes. As demonstrating examples, Cu/Ni-HHTP (HHTP: 2,3,6,7,10,11-hexahydroxytriphenylene) and Cu-BTPA (BTPA: benzene-1,3,5-triyltriboronic acid) are cathodically deposited on indium-doped tin oxide (ITO) glass substrates. The measured conductivity of these deposited conductive MOF films varies from 0.01 to 0.1 S cm-1 depending on their thickness and composition. Both of the fabricated conductive MOF films show good performance on supercapacitors and electrochemical sensing.

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Yildirim, Onur, Matteo Bonomo, Nadia Barbero, Cesare Atzori, Bartolomeo Civalleri, Francesca Bonino, Guido Viscardi und Claudia Barolo. „Application of Metal-Organic Frameworks and Covalent Organic Frameworks as (Photo)Active Material in Hybrid Photovoltaic Technologies“. Energies 13, Nr. 21 (26.10.2020): 5602. http://dx.doi.org/10.3390/en13215602.

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Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) are two innovative classes of porous coordination polymers. MOFs are three-dimensional materials made up of secondary building blocks comprised of metal ions/clusters and organic ligands whereas COFs are 2D or 3D highly porous organic solids made up by light elements (i.e., H, B, C, N, O). Both MOFs and COFs, being highly conjugated scaffolds, are very promising as photoactive materials for applications in photocatalysis and artificial photosynthesis because of their tunable electronic properties, high surface area, remarkable light and thermal stability, easy and relative low-cost synthesis, and structural versatility. These properties make them perfectly suitable for photovoltaic application: throughout this review, we summarize recent advances in the employment of both MOFs and COFs in emerging photovoltaics, namely dye-sensitized solar cells (DSSCs) organic photovoltaic (OPV) and perovskite solar cells (PSCs). MOFs are successfully implemented in DSSCs as photoanodic material or solid-state sensitizers and in PSCs mainly as hole or electron transporting materials. An innovative paradigm, in which the porous conductive polymer acts as standing-alone sensitized photoanode, is exploited too. Conversely, COFs are mostly implemented as photoactive material or as hole transporting material in PSCs.

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Wang, Shi, Ping Li, Junyi Wang, Jun Gong, Helin Lu, Xiaobo Wang, Quan Wang und Ping Xue. „Detection of Ascorbic Acid by Two-Dimensional Conductive Metal-Organic Framework-Based Electrochemical Sensors“. Molecules 29, Nr. 11 (21.05.2024): 2413. http://dx.doi.org/10.3390/molecules29112413.

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The realization of efficient and accurate detection of biomolecules has become a key scientific issue in the field of life sciences. With the rapid development of nanotechnology, electrochemical sensors constructed from the superior physical and chemical properties of nanomaterials show faster and more accurate detection. Among nanomaterials, two-dimensional conductive MOF (2D cMOF) is considered to be a star material in electrochemical sensors due to its remarkable conductivity, high porosity, and stability. In this paper, a Cu3(HHTP)2/SPE electrochemical sensor for the detection of ascorbic acid (AA) was constructed by modifying 2D cMOF (Cu3(HHTP)2) on the surface of the screen-printed electrode (SPE). The sensor exhibited excellent catalytic activity in the detection of AA, with a lower detection limit of 2.4 μmol/L (S/N = 3) and a wide linear range of 25–1645 μmol/L. This high catalytic activity can be attributed to the abundant catalytic sites in Cu3(HHTP)2 and the rapid electron transfer between Cu+ and Cu2+, which accelerates the oxidation of AA. This work lays a foundation for the subsequent development of MOFs with special electrochemical catalytic properties and the integration of 2D cMOF into intelligent electrical analysis devices.

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Nyakuchena, James, und James Nyakuchena. „(First Place Poster Award) Probing Charge Transport Mechanisms in 2D Metal Organic Frameworks“. ECS Meeting Abstracts MA2023-01, Nr. 17 (28.08.2023): 2825. http://dx.doi.org/10.1149/ma2023-01172825mtgabs.

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Metal Organic Frameworks (MOFs) are a class of highly porous crystalline materials that are constructed from zero- or one-dimensional inorganic chains in combination with multitopic organic ligands.1 They have received great attention recently due to their large surface area, tunable porosity, and easy preparation, which lead to their versatile applications including gas storage2 and separation3, sensing4, catalysis5 and drug delivery6. The versatility of MOFs is further entrenched in the vast available design space offered by the enormous number of metal-linker combinations7, 8. However, majority of MOFs are insulators with very few of them showing appreciable electrical conductivity. The insulating nature of MOFs can be traced back to the starting materials used in constructing these hybrid materials9. Although conductive MOFs have been reported, very little information about the mechanism of charge transport is available.10-12 There are mainly two types of charge transport mechanism reported in such materials, hopping and band transport.13 Hopping mechanism is dominated by movement of charges from donor to acceptor moieties due to charge localization which exists at specific sites within the MOF.13 Band transport relies on delocalization of carriers throughout the valence and conduction bands.14 These mechanisms require low energy pathways for charge transport which are not present in MOFs. Recently, researchers have focused on two synthetic approaches from a chemical perspective to achieve such low energy pathways; through bond approach and through space approach.13 Ideally, both pathways can either lead to band or hopping transport. The through space mechanism utilizes non-covalent interactions like π-π stacking between organic linkers, which creates an extended pathway for charge delocalization usually pronounced in 2D MOFs.15, 16 Recent studies which have successfully quantified and identified charge carrier types in MOFs17 show that conductivity increases mainly with chemical oxidation signifying hole formation18, but mobility and directional charge transfer is still limited by geometry.19 Although the field of electrically conductive MOFs has experienced tremendous expansion in the last decade and yielded a variety of MOFs with high mobility and conductivity, majority of these works focus on material design principle and conductivity measurement, leaving the fundamental understanding of CT mechanism underexplored; yet the latter is essential for the further development of this class of materials to be exploited in optoelectronics, solar cells, and photocatalysis. I will present my progress in exploring CT mechanisms in 2D MOFs using advanced spectroscopic techniques. References C. Janiak and J. K. Vieth, New J. Chem., 2010, 34, 2366-2388. M. Latroche, S. Surble, C. Serre, C. Mellot-Draznieks, P. L. Llewellyn, J. H. Lee, J. S. Chang, S. H. Jhung and G. Ferey, Angewandte Chemie-International Edition, 2006, 45, 8227-8231. Z. J. Zhang, Y. G. Zhao, Q. H. Gong, Z. Li and J. Li, Chem. Commun., 2013, 49, 653-661. E. A. Dolgopolova, A. M. Rice, C. R. Martin and N. B. Shustova, Chem. Soc. Rev., 2018, 47, 4710-4728. Y. X. Zhou, W. H. Hu, S. Z. Yang, Y. B. Zhang, J. Nyakuchena, K. Duisenova, S. Lee, D. H. Fan and J. Huang, Journal of Physical Chemistry C, 2020, 124, 1405-1412. I. A. Lazaro and R. S. Forgan, Coord. Chem. Rev., 2019, 380, 230-259. C. Muschielok and H. Oberhofer, J. Chem. Phys., 2019, 151. L. Sun, M. G. Campbell and M. Dinca, Angewandte Chemie-International Edition, 2016, 55, 3566-3579. P. F. Li and B. Wang, Isr. J. Chem., 2018, 58, 1010-1018. K. W. Nam, S. S. Park, R. dos Reis, V. P. Dravid, H. Kim, C. A. Mirkin and J. F. Stoddart, Nature Communications, 2019, 10, 10. T. Chen, J.-H. Dou, L. Yang, C. Sun, N. J. Libretto, G. Skorupskii, J. T. Miller and M. Dincă, J. Am. Chem. Soc., 2020, 142, 12367-12373. S. S. Park, E. R. Hontz, L. Sun, C. H. Hendon, A. Walsh, T. Van Voorhis and M. Dincă, J. Am. Chem. Soc., 2015, 137, 1774-1777. M. Ko, L. Mendecki and K. A. Mirica, Chem. Commun., 2018, 54, 7873-7891. R. Dong, P. Han, H. Arora, M. Ballabio, M. Karakus, Z. Zhang, C. Shekhar, P. Adler, P. St Petkov, A. Erbe, S. C. B. Mannsfeld, C. Felser, T. Heine, M. Bonn, X. L. Feng and E. Canovas, Nature Materials, 2018, 17, 1027-+. L. Y. Qu, H. Iguchi, S. Takaishi, F. Habib, C. F. Leong, D. M. D'Alessandro, T. Yoshida, H. Abe, E. Nishibori and M. Yamashita, J. Am. Chem. Soc., 2019, 141, 6802-6806. L. S. Xie, E. V. Alexandrov, G. Skorupskii, D. M. Proserpio and M. Dinca, Chemical Science, 2019, 10, 8558-8565.A. C. Hinckley, J. Park, J. Gomes, E. Carlson and Z. Bao, J. Am. Chem. Soc., 2020, 142, 11123-11130. S.

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Ye, Rui-Hong, Jin-Yang Chen, Di-Hui Huang, Yan-Jun Wang und Sheng Chen. „Electrochemical Sensor Based on Glassy-Carbon Electrode Modified with Dual-Ligand EC-MOFs Supported on rGO for BPA“. Biosensors 12, Nr. 6 (27.05.2022): 367. http://dx.doi.org/10.3390/bios12060367.

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The electronic conductive metal-organic frameworks (EC-MOFs) based on a single ligand are not suitable for the accurate detection of bisphenol A (BPA) due to the limitations of their electron-transfer-based sensing mechanism. To overcome this drawback, we developed EC-MOFs with novel dual-ligands, 2,3,6,7,10,11-hexahydroxy-sanya-phenyl (HHTP) and tetrahydroxy 1,4-quinone (THQ), and metal ions. A new class of 2D π-conjugation-based EC-MOFs (M-(HHTP)(THQ)) was synthesized by a self-assemble technique. Its best member (Cu-(HHTP)(THQ)) was selected and combined with reduced graphene (rGO) to form a Cu-(HHTP)(THQ)@rGO composite, which was thoroughly characterized by X-ray diffraction, field scanning electron microscopy, and energy-dispersive X-ray spectroscopy. Cu-(HHTP)(THQ)@rGO was drop-cast onto a glassy carbon electrode (GCE) to obtain a sensor for BPA detection. Cyclic voltammetry and electrochemical impedance tests were used to evaluate the electrode performance. The oxidation current of BPA on the Cu-(HHTP)(THQ)@rGO/GCE was substantially higher than on unmodified GCE, which could be explained by a synergy between Cu-(HHTP)(THQ) (which provided sensing and adsorption) and rGO (which provided fast electron conductivity and high surface area). Cu-(HHTP)(THQ)@rGO/GCE exhibited a linear detection range for 0.05–100 μmol·L−1 of BPA with 3.6 nmol·L−1 (S/N = 3) detection limit. We believe that our novel electrode and BPA sensing method extends the application perspectives of EC-MOFs in the electrocatalysis and sensing fields.

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Cánovas, Enrique. „(Invited) Record-High Charge Carrier Mobilities in 2D Covalent- and Metal- Organic Frameworks“. ECS Meeting Abstracts MA2023-01, Nr. 11 (28.08.2023): 1235. http://dx.doi.org/10.1149/ma2023-01111235mtgabs.

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Organic based 2D layered materials (2DLMs) including 2D covalent and metal organic frameworks (COFs and MOFs) are promising candidates for traditional applications in gas storage and separation as well as catalysis. This is due to the long-range crystalline order that can be achieved in them as well as their tunable porosity and chemistry. Synthetic chemistry efforts aiming an enhanced coupling between their building block constituents have recently led to the design of (semi-)conducting MOFs and COFs displaying high conductivities and record charge carrier mobilities. These achievements have opened the path for their application in opto-electronics. Yet, despite being a critical aspect for the development of 2DLM based electronics, understanding the true nature of charge transport in these novel materials by stabilising reliable structure-property-function relations is largely unexplored. Here I will present time-resolved high-frequency (terahertz) conductivity studies of state-of-the-art organic based 2DLMs materials revealing semiconducting behaviour and record charge carrier mobilities. First, I will present a detailed characterization for the electronic properties of Zn– and Cu–phthalocyanine-based pyrazine-linked 2D COFs [1,2]. These 2D COFs, synthesized by condensation of metal–phthalocyanine (M = Zn and Cu) and pyrene derivatives, are obtained as polycrystalline-layered semiconductors displaying p-type doping and a band gap of ∼1.2 eV. Hall effect measurements (dc limit) and terahertz (THz) spectroscopy (ac limit) in combination with density functional theory (DFT) calculations demonstrate that varying metal center from Cu to Zn in the phthalocyanine moiety has a negligible effect in the conductivity (∼5 × 10–7 S/cm), charge carrier density (∼1012 cm–3), charge carrier scattering rate (∼3 × 1013 s–1), and effective mass (∼2.3m0) of majority carriers (holes). However, both samples reveal slightly different mobilities that can be attributed to charge carrier localization at crystalline grain boundaries. Furthermore we analyse the effect of iodine doping on the Zn based 2D COFs. The resultant 2D c-COF ZnPc-pz-I2 maintains its structural integrity and displays enhanced conductivity by 3 orders of magnitude, as a result of improved charge carrier concentrations. Hall effect reveal a charge carrier mobility reaching ∼22 cm2/Vs for ZnPc-pz-I2, which represent a record value for 2D c-COFs. An improved mobility upon doping can be traced to an increase in scattering time for free charge carriers, indicating that scattering mechanisms limiting the mobility are mitigated by doping. In the second part of my talk, I present the results concerning a Fe3(THT)2 (THT=2,3,6,7,10,11-hexathioltriphenylene) 2D MOFs [3]. The π-d conjugated samples, synthesized through interfacial method at room temperature, are obtained as a large-area, free-standing films with tunable geometry (size and thickness). The Fe3(THT)2 films are porous (specific surface area of 526±5 m2/g) and semiconducting (with a ~250 meV direct bandgap), and remarkably display band-like charge transport. This finding is directly demonstrated from the Drude-type high-frequency (terahertz) photo-conductivity response obtained in the samples; revealing free-moving, delocalized charge carriers displaying ~220 cm2/Vs mobilities at room temperature; a record charge carrier mobility for MOFs. The temperature dependence of the mobility reveals that the main scattering mechanism limiting the mobility and hence band-like charge transport in this material is related to impurity scattering, so that material improvements may further increase the mobility. The demonstration of band-like charge transport and record-high mobilities in semiconducting 2D COFs and MOFs reveal the potential of (porous) electrically conductive 2DLMs to be employed as active materials in opto-electronics devices. References: [1] “Unveiling electronic properties in metal-phthalocyanine-based pyrazine-linked conjugated two-dimensional colvalent organic frameworks” Mingchao Wang, Marco Ballabio, Mao Wang, Hung-Hsuan Lin, Bishnu Prasad Biswal, Xiaocang Han, Silvia Paasch, Eike Brunner, Pan Liu, Mingwei Chen, Mischa Bonn, Thomas Heine, Shengqiang Zhou, Enrique Canovas*, Renhao Dong*, Xinliang Feng*, JACS 141, 16810-16816, 2019. [2] “High-Mobility Semiconducting Two-Dimensional Conjugated Covalent Organic Frameworks with p-Type Doping” Mingchao Wang, Mao Wang, Hung-Hsuan Lin, Marco Ballabio, Haixia Zhong, Mischa Bonn, Shengqiang Zhou, Thomas Heine, Enrique Cánovas*, Renhao Dong*, Xinliang Feng*, JACS 142, 21622-21627, 2020. [3] “High-mobility band-like charge transport in a semiconducting two-dimensional metal–organic framework” Renhao Dong#, Peng Han#, Himani Arora, Marco Ballabio, Melike Karakus, Zhe Zhang, Chandra Shekhar, Peter Adler, Petko St. Petkov, Artur Erbe, Stefan C. B. Mannsfeld, Claudia Felser, Thomas Heine, Mischa Bonn, Xinliang Feng* & Enrique Cánovas* Nature Materials 17, 1027-1032 (2018)

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Meng, Chunfeng, Pinfei Hu, Hantao Chen, Yueji Cai, Hu Zhou, Zehong Jiang, Xiang Zhu, Zeyu Liu, Chengyin Wang und Aihua Yuan. „2D conductive MOFs with sufficient redox sites: reduced graphene oxide/Cu-benzenehexathiolate composites as high capacity anode materials for lithium-ion batteries“. Nanoscale 13, Nr. 16 (2021): 7751–60. http://dx.doi.org/10.1039/d0nr08549a.

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Qin, Yin, Ming-Hao Xue, Bao-Heng Dou, Zhi-Bing Sun und Gang Li. „High protonic conduction in two metal–organic frameworks containing high-density carboxylic groups“. New Journal of Chemistry 44, Nr. 7 (2020): 2741–48. http://dx.doi.org/10.1039/c9nj05735h.

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Itakura, Tomoya, Hiroshi Matsui, Tomofumi Tada, Susumu Kitagawa, Aude Demessence und Satoshi Horike. „The role of lattice vibration in the terahertz region for proton conduction in 2D metal–organic frameworks“. Chemical Science 11, Nr. 6 (2020): 1538–41. http://dx.doi.org/10.1039/c9sc05757a.

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Haroon, Naila, und Keith J. Stine. „Electrochemical Detection of Hormones Using Nanostructured Electrodes“. Coatings 13, Nr. 12 (04.12.2023): 2040. http://dx.doi.org/10.3390/coatings13122040.

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Hormones regulate several physiological processes in living organisms, and their detection requires accuracy and sensitivity. Recent advances in nanostructured electrodes for the electrochemical detection of hormones are described. Nanostructured electrodes’ high surface area, electrocatalytic activity, and sensitivity make them a strong hormone detection platform. This paper covers nanostructured electrode design and production using MOFs, zeolites, carbon nanotubes, metal nanoparticles, and 2D materials such as TMDs, Mxenes, graphene, and conducting polymers onto electrodes surfaces that have been used to confer distinct characteristics for the purpose of electrochemical hormone detection. The use of aptamers for hormone recognition is producing especially promising results, as is the use of carbon-based nanomaterials in composite electrodes. These materials are optimized for hormone detection, allowing trace-level quantification. Various electrochemical techniques such as SWV, CV, DPV, EIS, and amperometry are reviewed in depth for hormone detection, showing the ability for quick, selective, and quantitative evaluation. We also discuss hormone immobilization on nanostructured electrodes to improve detection stability and specificity. We focus on real-time monitoring and tailored healthcare with nanostructured electrode-based hormone detection in clinical diagnostics, wearable devices, and point-of-care testing. These nanostructured electrode-based assays are useful for endocrinology research and hormone-related disease diagnostics due to their sensitivity, selectivity, and repeatability. We conclude with nanotechnology–microfluidics integration and tiny portable hormone-detection devices. Nanostructured electrodes can improve hormone regulation and healthcare by facilitating early disease diagnosis and customized therapy.

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Yang, Mingyu, Yi Zhang, Renlong Zhu, Junjun Tan, Jinxin Liu, Wei Zhang, Meng Zhou und Zheng Meng. „Two‐Dimensional Conjugated Metal–Organic Frameworks with a Ring‐in‐Ring Topology and High Electrical Conductance“. Angewandte Chemie International Edition, 16.04.2024. http://dx.doi.org/10.1002/anie.202405333.

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Electrically conducting two‐dimensional (2D) metal‐organic frameworks (MOFs) have garnered significant interest due to their remarkable structural tunability and outstanding electrical properties. However, the design and synthesis of high‐performance materials face challenges due to the limited availability of specific ligands and pore structures. In this study, we have employed a novel highly branched D3h symmetrical planar conjugated ligand, dodechydroxylhexabenzotrinaphthylene (DHHBTN) to fabricate a series of 2D conductive MOFs, named M‐DHHBTN (M = Co, Ni, and Cu). This new family of MOFs offers two distinct types of pores, elevating the structural complexity of 2D conductive MOFs to a more advanced level. The intricate tessellation patterns of the M‐DHHBTN are elucidated through comprehensive analyses involving powder X‐ray diffraction, theoretical simulations, and high‐resolution transmission electron microscope. Optical‐pump terahertz‐probe spectroscopic measurements unveiled carrier mobility in DHHBTN‐based 2D MOFs spanning from 0.69 to 3.10 cm2 V‐1 s‐1. Among M‐DHHBTN famility, Cu‐DHHBTN displayed high electrical conductivity reaching 0.21 S cm−1 at 298 K with thermal activation behavior. This work leverages the “branched conjugation” of the ligand to encode heteroporosity into highly conductive 2D MOFs, underscoring the significant potential of heterogeneous double‐pore structures for future applications.

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Yang, Mingyu, Yi Zhang, Renlong Zhu, Junjun Tan, Jinxin Liu, Wei Zhang, Meng Zhou und Zheng Meng. „Two‐Dimensional Conjugated Metal–Organic Frameworks with a Ring‐in‐Ring Topology and High Electrical Conductance“. Angewandte Chemie, April 2024. http://dx.doi.org/10.1002/ange.202405333.

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Electrically conducting two‐dimensional (2D) metal‐organic frameworks (MOFs) have garnered significant interest due to their remarkable structural tunability and outstanding electrical properties. However, the design and synthesis of high‐performance materials face challenges due to the limited availability of specific ligands and pore structures. In this study, we have employed a novel highly branched D3h symmetrical planar conjugated ligand, dodechydroxylhexabenzotrinaphthylene (DHHBTN) to fabricate a series of 2D conductive MOFs, named M‐DHHBTN (M = Co, Ni, and Cu). This new family of MOFs offers two distinct types of pores, elevating the structural complexity of 2D conductive MOFs to a more advanced level. The intricate tessellation patterns of the M‐DHHBTN are elucidated through comprehensive analyses involving powder X‐ray diffraction, theoretical simulations, and high‐resolution transmission electron microscope. Optical‐pump terahertz‐probe spectroscopic measurements unveiled carrier mobility in DHHBTN‐based 2D MOFs spanning from 0.69 to 3.10 cm2 V‐1 s‐1. Among M‐DHHBTN famility, Cu‐DHHBTN displayed high electrical conductivity reaching 0.21 S cm−1 at 298 K with thermal activation behavior. This work leverages the “branched conjugation” of the ligand to encode heteroporosity into highly conductive 2D MOFs, underscoring the significant potential of heterogeneous double‐pore structures for future applications.

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Shoaib Ahmad Shah, Syed, Muhammad Altaf Nazir, Azhar Mahmood, Manzar Sohail, Aziz ur Rehman, Muhammad Khurram Tufail, Tayyaba Najam et al. „Synthesis of Electrical Conductive Metal‐Organic Frameworks for Elelctrochemical Applications“. Chemical Record, 18.09.2023. http://dx.doi.org/10.1002/tcr.202300141.

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AbstractElectrical conductivity is very important property of nanomaterials for using wide range of applications especially energy applications. Metal‐organic frameworks (MOFs) are notorious for their low electrical conductivity and less considered for usage in pristine forms. However, the advantages of high surface area, porosity and confined catalytic active sites motivated researchers to improve the conductivity of MOFs. Therefore, 2D electrical conductive MOFs (ECMOF) have been widely synthesized by developing the effective synthetic strategies. In this article, we have summarized the recent trends in developing the 2D ECMOFs, following the summary of potential applications in the various fields with future perspectives.

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Huang, Chuanhui, Weiming Sun, Yingxue Jin, Quanquan Guo, David Mücke, Xingyuan Chu, Zhongquan Liao et al. „A General Synthesis of Nanostructured Conductive MOFs from Insulating MOF Precursors for Supercapacitors and Chemiresistive Sensors“. Angewandte Chemie, 27.11.2023. http://dx.doi.org/10.1002/ange.202313591.

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Two‐dimensional conjugated metal‐organic frameworks (2D c‐MOFs) are emerging as unique layer‐stacked crystalline coordination polymers that simultaneously possess porous and conductive properties. However, the controlled synthesis of hierarchically nanostructured 2D c‐MOFs with high crystallinity and customized morphologies is essential for energy and electronic devices, which remains a great challenge. Herein, we present a template strategy to synthesize 12 different 2D c‐MOFs with controlled morphologies and dimensions via insulating MOFs‐to‐c‐MOFs transformations. The resultant hierarchically nanostructured 2D c‐MOFs feature intrinsic electrical conductivity (up to 102 S cm‐1) and higher surface areas (up to ~62 times) than the reported bulk‐type 2D c‐MOFs, which are beneficial for improved access to active sites and enhanced mass transport. As proof‐of‐concept applications, the resultant hollow Cu‐BHT nanocube‐based supercapacitor exhibits over 2.3‐fold improvement in specific capacity (364.5 F g‐1) in organic electrolyte than the bulk‐type Cu‐BHT (161.9 F g‐1), surpassing the reported MOF‐based electrodes (up to 202 F g‐1). In addition, the Cu‐HHB nanoflower‐based chemiresistive gas sensor displays over 2.5‐fold enhancement in response intensity toward H2S compared to bulk‐type Cu‐HHB, boasting the fastest response speed and one of the lowest limits of detection ever reported for H2S sensors at room temperature.

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Huang, Chuanhui, Weiming Sun, Yingxue Jin, Quanquan Guo, David Mücke, Xingyuan Chu, Zhongquan Liao et al. „A General Synthesis of Nanostructured Conductive MOFs from Insulating MOF Precursors for Supercapacitors and Chemiresistive Sensors“. Angewandte Chemie International Edition, 27.11.2023. http://dx.doi.org/10.1002/anie.202313591.

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Two‐dimensional conjugated metal‐organic frameworks (2D c‐MOFs) are emerging as unique layer‐stacked crystalline coordination polymers that simultaneously possess porous and conductive properties. However, the controlled synthesis of hierarchically nanostructured 2D c‐MOFs with high crystallinity and customized morphologies is essential for energy and electronic devices, which remains a great challenge. Herein, we present a template strategy to synthesize 12 different 2D c‐MOFs with controlled morphologies and dimensions via insulating MOFs‐to‐c‐MOFs transformations. The resultant hierarchically nanostructured 2D c‐MOFs feature intrinsic electrical conductivity (up to 102 S cm‐1) and higher surface areas (up to ~62 times) than the reported bulk‐type 2D c‐MOFs, which are beneficial for improved access to active sites and enhanced mass transport. As proof‐of‐concept applications, the resultant hollow Cu‐BHT nanocube‐based supercapacitor exhibits over 2.3‐fold improvement in specific capacity (364.5 F g‐1) in organic electrolyte than the bulk‐type Cu‐BHT (161.9 F g‐1), surpassing the reported MOF‐based electrodes (up to 202 F g‐1). In addition, the Cu‐HHB nanoflower‐based chemiresistive gas sensor displays over 2.5‐fold enhancement in response intensity toward H2S compared to bulk‐type Cu‐HHB, boasting the fastest response speed and one of the lowest limits of detection ever reported for H2S sensors at room temperature.

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Chang, Zixin, Mengsu Zhu, Ze Li, Sha Wu, Siping Yin, Yimeng Sun und Wei Xu. „2D Conductive Metal‐Organic Frameworks Based on Tetraoxa[8]circulenes as Promising Cathode for Aqueous Zinc Ion Batteries“. Small, 08.03.2024. http://dx.doi.org/10.1002/smll.202400923.

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AbstractAqueous zinc‐ion batteries (ZIBs) are the new generation electrochemical energy storage systems. Recently, two‐dimensional conductive metal‐organic frameworks (2D c‐MOFs) are attractive to serve as cathode materials of ZIBs due to their compositional diversity, abundant active sites, and excellent conductivity. Despite the growing interest in 2D c‐MOFs, their application prospects are still to be explored. Herein, a tetraoxa[8]circulene (TOC) derivative with unique electronic structure and interesting redox‐active property are synthesized to construct c‐MOFs. A series of novel 2D c‐MOFs (Cu‐TOC, Zn‐TOC and Mn‐TOC) with different conductivities and packing modes are obtained by combining the linker tetraoxa[8]circulenes‐2,3,5,6,8,9,11,12‐octaol (8OH‐TOC) and corresponding metal ions. Three c‐MOFs all exhibit typical semiconducting properties, and Cu‐TOC exhibits the highest electrical conductivity of 0.2 S cm−1 among them. Furthermore, their electrochemical performance as cathode materials for ZIBs have been investigated. They all performed high reversible capacity, decent cycle stability and excellent rate capability. This work reveals the key insights into the electrochemical application potential of 2D c‐MOFs and advances their development as cathode materials in ZIBs.

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Lu, Yang, Yingying Zhang, Chi-Yuan Yang, Sergio Revuelta, Haoyuan Qi, Chuanhui Huang, Wenlong Jin et al. „Precise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks“. Nature Communications 13, Nr. 1 (24.11.2022). http://dx.doi.org/10.1038/s41467-022-34820-6.

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AbstractTwo-dimensional conjugated metal-organic frameworks (2D c-MOFs) have attracted increasing interests for (opto)-electronics and spintronics. They generally consist of van der Waals stacked layers and exhibit layer-depended electronic properties. While considerable efforts have been made to regulate the charge transport within a layer, precise control of electronic coupling between layers has not yet been achieved. Herein, we report a strategy to precisely tune interlayer charge transport in 2D c-MOFs via side-chain induced control of the layer spacing. We design hexaiminotriindole ligands allowing programmed functionalization with tailored alkyl chains (HATI_CX, X = 1,3,4; X refers to the carbon numbers of the alkyl chains) for the synthesis of semiconducting Ni3(HATI_CX)2. The layer spacing of these MOFs can be precisely varied from 3.40 to 3.70 Å, leading to widened band gap, suppressed carrier mobilities, and significant improvement of the Seebeck coefficient. With this demonstration, we further achieve a record-high thermoelectric power factor of 68 ± 3 nW m−1 K−2 in Ni3(HATI_C3)2, superior to the reported holes-dominated MOFs.

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Li, Jiawen, Peng Liu, Jianxin Mao, Jianyue Yan und Wenbo Song. „Two-dimensional conductive metal–organic frameworks with dual metal sites toward the electrochemical oxygen evolution reaction“. Journal of Materials Chemistry A, 2021. http://dx.doi.org/10.1039/d0ta10870g.

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27

Liu, Xiaobin, Mengxiao Yu, Jiaqiang Liu, Songgu Wu und Junbo Gong. „A Triptycene‐Based Layered/Flower‐Like 2D Conductive Metal–Organic Framework with 3D Extension as an Electrode for Efficient Li Storage“. Small, 15.10.2023. http://dx.doi.org/10.1002/smll.202306159.

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Abstract2D metal–organic frameworks (2D MOFs) with π conjugation have attracted widespread attention in the field of lithium storage due to their unique electron transfer units and structural characteristics. However, the periodic 2D planar extension structure hides some active sites, which is not conducive to the utilization of its structural advantages. In this work, a series of triptycene‐based 2D conductive MOFs (M‐DBH, M = Ni, Mn, and Co) with 3D extension structures are constructed by coordinating 9,10‐dihydro‐9,10‐[1,2]benzenoanthracene‐2,3,6,7,14,15‐hexaol with metal ions to explore their potential applications in lithium‐ion and lithium–sulfur batteries. This is the first study in which 2D conductive MOFs with the 3D extended molecule are used as electrode materials for lithium storage. The designed material generates rich active sites through staggered stacking layers and shows excellent performance in lithium‐ion and lithium–sulfur batteries. The capacity retention rate of Ni‐DBH can reach over 70% after 500 cycles at 0.2 C in lithium‐ion batteries, while the capacity of S@Mn‐DBH exceeds 305 mAh g−1 after 480 cycles at 0.5 C in lithium–sulfur batteries. Compared with the materials with 2D planar extended structures, the M‐DBH electrodes with 3D extended structures in this work exhibit better performance in terms of cycle time and lithium storage capacity.

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Zhang, Qi, Pingao Hu, Zhi-Yuan Xu, Bei-Bei Tang, Huiru Zhang, Yuhong Xiao und Yucheng Wu. „Unravelling intrinsic descriptor based on two-stage activity regulation of bimetallic 2D c-MOFs for CO2RR“. Nanoscale, 2023. http://dx.doi.org/10.1039/d2nr07301c.

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The bimetallic 2D conductive MOFs of M1Pc-M2-O, possessing dual metal sites to realize flexible molecular level structural modification, are brilliant catalysts for electrochemical CO2 reduction. However, the bimetallic centers bring...

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Shin, Sun Hae Ra, Jinhui Tao, Nathan L. Canfield, Mark E. Bowden, Lili Liu, Bhuvaneswari M. Sivakumar, Jun Liu, James J. De Yoreo, Praveen K. Thallapally und Maria L. Sushko. „Role of Solvent in the Oriented Growth of Conductive Ni‐CAT‐1 Metal‐Organic Framework at Solid–Liquid Interfaces“. Advanced Materials Interfaces, 02.04.2024. http://dx.doi.org/10.1002/admi.202301009.

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AbstractA controlled growth of two‐dimensional (2D) π‐conjugated metal‐organic frameworks (MOFs) on solid substrates can open exciting opportunities for the application of 2D MOFs as optoelectronic devices. Some factors like solvent composition and type of substrates are known to influence the properties of solution‐processed 2D MOF crystals; however, a mechanistic understanding of how interactions between solvent, substrate, and precursors affect heterogeneous nucleation has been limited. Here, it is reported that the structure of Ni‐catecholate (Ni‐CAT‐1) MOFs at a solid–liquid interface is controlled by solvent–substrate and solvent–MOF precursor interactions. Specifically, the structure of the MOF film can be controlled by varying the affinity of the solvent to the substrate. As a fraction of N,N‐dimethylformamide (DMF) in a binary solvent mixture of water and DMF increases, the arrangement of Ni‐CAT‐1 crystals varies from vertically aligned nanorods to the graphite substrate to less ordered nanorods with the lower initial nucleation number density of Ni‐CAT‐1 crystals on the surface.

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Ahmad, Ali, Muhammad Faisal Nadeem, Kashif Elahi und Roslan Hasni. „Computing topological indices of chemical structures of the conductive 2D MOFs“. Journal of Information and Optimization Sciences, 07.07.2020, 1–16. http://dx.doi.org/10.1080/02522667.2020.1773021.

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31

Song, Jiajun, Hong Liu, Zeyu Zhao, Xuyun Guo, Chun-ki Liu, Sophie Griggs, Adam Marks et al. „2D metal-organic frameworks for ultraflexible electrochemical transistors with high transconductance and fast response speeds“. Science Advances 9, Nr. 2 (13.01.2023). http://dx.doi.org/10.1126/sciadv.add9627.

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Electrochemical transistors (ECTs) have shown broad applications in bioelectronics and neuromorphic devices due to their high transconductance, low working voltage, and versatile device design. To further improve the device performance, semiconductor materials with both high carrier mobilities and large capacitances in electrolytes are needed. Here, we demonstrate ECTs based on highly oriented two-dimensional conjugated metal-organic frameworks (2D c-MOFs). The ion-conductive vertical nanopores formed within the 2D c-MOFs films lead to the most convenient ion transfer in the bulk and high volumetric capacitance, endowing the devices with fast speeds and ultrahigh transconductance. Ultraflexible device arrays are successfully used for wearable on-skin recording of electrocardiogram (ECG) signals along different directions, which can provide various waveforms comparable with those of multilead ECG measurement systems for monitoring heart conditions. These results indicate that 2D c-MOFs are excellent semiconductor materials for high-performance ECTs with promising applications in flexible and wearable electronics.

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Liu, Jingjuan, Yi Zhou, Guolong Xing, Meiling Qi, Zhe Tang, Osamu Terasaki und Long Chen. „2D Conductive Metal–Organic Framework with Anthraquinone Built‐In Active Sites as Cathode for Aqueous Zinc Ion Battery“. Advanced Functional Materials, 30.01.2024. http://dx.doi.org/10.1002/adfm.202312636.

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Abstract2D conductive metal–organic frameworks (2D c‐MOFs) as emerging 2D graphene‐like crystalline materials have become a promising platform for energy storage. However, their capacity is largely constrained by the limited number of electroactive sites. Integrating multiple redox‐active moieties into the 2D c‐MOF skeletons is an efficient strategy toward high‐performance battery cathodes. Herein, by tailoring an anthraquinone‐based multitopic catechol ligand, a novel quinone‐containing copper‐catecholate MOF (Cu‐TBPQ MOF) is successfully developed. The Cu‐TBPQ MOF exhibits abundant porosity, excellent conductivity, and multiple redox‐active sites. These characteristics make it an ideal candidate as a cathode material for zinc ion batteries. Notably, the Cu‐TBPQ MOF demonstrates an impressive reversible specific capacity of 371.2 mAh g−1 at a current density of 50 mA g−1. Furthermore, it exhibits outstanding rate capability and long‐term durability, retaining a capacity of 120.3 mAh g−1 at a high current density of 2.0 A g−1 even after 500 charge–discharge cycles. The successful enrichment of redox‐active sites in the work opens up new avenues for the rational design of electrochemically active 2D c‐MOFs, enhancing their potential for advanced energy storage applications.

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Zu, Shu, Huan Zhang, Tong Zhang, Mingdao Zhang und Li Song. „Ni–Rh-based bimetallic conductive MOF as a high-performance electrocatalyst for the oxygen evolution reaction“. Frontiers in Chemistry 11 (29.09.2023). http://dx.doi.org/10.3389/fchem.2023.1242672.

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Metal–organic frameworks (MOFs) have recently been considered the promising catalysts due to their merits of abundant metal sites, versatile coordination groups, and tunable porous structure. However, low electronic conductivity of most MOFs obstructs their direct application in electrocatalysis. In this work, we fabricate an Ni–Rh bimetallic conductive MOF ([Ni2.85Rh0.15(HHTP)2]n/CC) grown in situ on carbon cloth. Abundant nanopores in the conductive MOFs expose additional catalytic active sites, and the advantageous 2D π-conjugated structure helps accelerate charge transfer. Owing to the introduction of Rh, [Ni2.85Rh0.15(HHTP)2]n/CC exhibited substantially improved oxygen evolution reaction (OER) activity and exhibited only an overpotential of 320 mV to achieve the current density of 20 mA cm-2. The remarkable OER performance confirmed by the electrochemical tests could be ascribed to the synergistic effect caused by the doped Rh together with Ni in [Ni2.85Rh0.15(HHTP)2]n/CC, thereby exhibiting outstanding electrocatalytic performance.

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Lin, Lingtong, Caiyun Zhang, Liwen Yin, Yuewen Sun, Danning Xing, Yuanyuan Liu, Peng Wang et al. „A Conductive 3D Dual‐Metal π‐d Conjugated Metal–Organic Framework Fe₃(HITP)₂/bpm@Co for Highly Efficient Oxygen Evolution Reaction“. Small, 22.12.2023. http://dx.doi.org/10.1002/smll.202309256.

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AbstractAlthough 2D π‐d conjugated metal–organic frameworks (MOFs) exhibit high in‐plane conductivity, the closely stacked layers result in low specific surface area and difficulty in mass transfer and diffusion. Hence, a conductive 3D MOF Fe3(HITP)2/bpm@Co (HITP = 2,3,6,7,10,11‐hexaiminotriphenylene) is reported through inserting bpm (4,4′‐bipyrimidine) ligands and Co2+ into the interlayers of 2D MOF Fe3(HITP)2. Compared to 2D Fe3(HITP)2 (37.23 m2 g−1), 3D Fe3(HITP)2/bpm@Co displays a huge improvement in the specific surface area (373.82 m2 g−1). Furthermore, the combined experimental and density functional theory (DFT) theoretical calculations demonstrate the metallic behavior of Fe3(HITP)2/bpm@Co, which will benefit to the electrocatalytic activity of it. Impressively, Fe3(HITP)2/bpm@Co exhibits prominent and stable oxygen evolution reaction (OER) performance (an overpotential of 299 mV vs RHE at a current density of 10 mA cm−2 and a Tafel slope of 37.14 mV dec−1), which is superior to 2D Fe3(HITP)2 and comparable to commercial IrO2. DFT theoretical calculation reveals that the combined action of the Fe and Co sites in Fe3(HITP)2/bpm@Co is responsible for the enhanced electrocatalytic activity. This work provides an alternative approach to develop conductive 3D MOFs as efficient electrocatalysts.

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Yin, Jia‐Cheng, Xin Lian, Zhi‐Gang Li, Mingren Cheng, Ming Liu, Jian Xu, Wei Li, Yunhua Xu, Na Li und Xian‐He Bu. „Triazacoronene‐Based 2D Conductive Metal–Organic Framework for High‐Capacity Lithium Storage“. Advanced Functional Materials, 12.04.2024. http://dx.doi.org/10.1002/adfm.202403656.

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Abstract2D conductive metal–organic frameworks (2D c‐MOFs) have attracted increasing attention as promising electrode materials for rechargeable batteries due to their designable periodic motifs, large specific surface areas, and prominent electrical conductivity. However, the development of 2D c‐MOF electrode materials with functionality remains a significant challenge because of the limited electroactive ligand motifs available. Herein, a hexahydroxy‐substituted triazacoronene ligand (6OH‐TAC) is deliberately designed and synthesized, which coordinates with Cu2+ ions to form an unprecedented 2D c‐MOF (Cu‐TAC) with functionality sites of efficient lithium storage. The synergistic effect of TAC and CuO4 enables Cu‐TAC as an anode for lithium‐ion batteries with a superior reversible capacity of 772.4 mAh g−1 at 300 mA g−1, remarkable rate performance, and outstanding long‐term cyclability (83% capacity retention at 300 mA g−1 for 600 cycles). These metrics outperform almost all 2D c‐MOF‐based electrodes, shedding light on new opportunities for energy storage devices.

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Xu, Wensi, Xiansen He, xiaokun Li und Suxiang Feng. „Electrochemical Sensor Based on Au NPs@NiPc-Cu MOFs Modified Electrode for the Rapid Detection of Luteolin“. Journal of The Electrochemical Society, 05.08.2022. http://dx.doi.org/10.1149/1945-7111/ac876a.

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Abstract In this study, a novel electrochemical sensor was designed to detect luteolin (Lu) with the composite of gold nanoparticles and nickel phthalocyanine-based 2D conductive metal-organic frameworks (Au NPs@NiPc-Cu MOFs) for the first time. The NiPc-Cu MOFs exhibit excellent conductivity, large specific surface area, and porous structure, which can accelerate the mass transfer process of target molecules. To further improve the sensitivity of the sensing platform, Au NPs with outstanding conductivity were introduced to the surface of NiPc-Cu MOFs to prepare Au NPs@NiPc-Cu MOFs. The synergistic effect of NiPc-Cu MOFs and Au NPs endows the sensor with excellent electrocatalytic performance and outstanding sensitivity. Under optimal conditions, the electrochemical sensor has a wide linear range (0.1-40 μM). Moreover, the prepared sensor possesses good stability and anti-interference ability. This method does not require complicated sample pretreatment, simple operation, and short detection time, which can provide a new method for the rapid detection of Lu.

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Wang, Denan, Sarah Ostresh, Daniel Streater, Peilei He, James Nyakuchena, Qiushi Ma, Xiaoyi Zhang, Jens Neu, Gary W. Brudvig und Jier Huang. „Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal‐Organic Frameworks“. Angewandte Chemie, 23.10.2023. http://dx.doi.org/10.1002/ange.202309505.

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Metal‐organic frameworks (MOFs) with mobile charges have attracted significant attention due to their potential applications in photoelectric devices, chemical resistance sensors, and catalysis. However, fundamental understanding of the charge transport pathway within the framework and the key properties that determine the performance of conductive MOFs in photoelectric devices remain underexplored. Herein, we report the mechanisms of photoinduced charge transport and electron dynamics in the conductive 2D M‐HHTP (M=Cu, Zn or Cu/Zn mixed; HHTP=2,3,6,7,10,11‐hexahydroxytriphenylene) MOFs and their correlation with photoconductivity using the combination of time‐resolved terahertz spectroscopy, optical transient absorption spectroscopy, X‐ray transient absorption spectroscopy, and density functional theory (DFT) calculations. We identify the through‐space hole transport mechanism through the interlayer sheet π‐π interaction, where photoinduced hole state resides in HHTP ligand and electronic state is localized at the metal center. Moreover, the photoconductivity of the Cu‐HHTP MOF is found to be 65.5 S•m‐1, which represents the record high photoconductivity for porous MOF materials based on catecholate ligands.

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Wang, Denan, Sarah Ostresh, Daniel Streater, Peilei He, James Nyakuchena, Qiushi Ma, Xiaoyi Zhang, Jens Neu, Gary W. Brudvig und Jier Huang. „Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal‐Organic Frameworks“. Angewandte Chemie International Edition, 23.10.2023. http://dx.doi.org/10.1002/anie.202309505.

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Metal‐organic frameworks (MOFs) with mobile charges have attracted significant attention due to their potential applications in photoelectric devices, chemical resistance sensors, and catalysis. However, fundamental understanding of the charge transport pathway within the framework and the key properties that determine the performance of conductive MOFs in photoelectric devices remain underexplored. Herein, we report the mechanisms of photoinduced charge transport and electron dynamics in the conductive 2D M‐HHTP (M=Cu, Zn or Cu/Zn mixed; HHTP=2,3,6,7,10,11‐hexahydroxytriphenylene) MOFs and their correlation with photoconductivity using the combination of time‐resolved terahertz spectroscopy, optical transient absorption spectroscopy, X‐ray transient absorption spectroscopy, and density functional theory (DFT) calculations. We identify the through‐space hole transport mechanism through the interlayer sheet π‐π interaction, where photoinduced hole state resides in HHTP ligand and electronic state is localized at the metal center. Moreover, the photoconductivity of the Cu‐HHTP MOF is found to be 65.5 S•m‐1, which represents the record high photoconductivity for porous MOF materials based on catecholate ligands.

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Efimova, Anastasiia S., Pavel V. Alekseevskiy, Maria V. Timofeeva, Yuliya A. Kenzhebayeva, Alina O. Kuleshova, Irina G. Koryakina, Dmitry I. Pavlov et al. „Exfoliation of 2D Metal‐Organic Frameworks: toward Advanced Scalable Materials for Optical Sensing“. Small Methods, 13.09.2023. http://dx.doi.org/10.1002/smtd.202300752.

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AbstractTwo‐dimensional metal‐organic frameworks (MOFs) occupy a special place among the large family of functional 2D materials. Even at a monolayer level, 2D MOFs exhibit unique sensing, separation, catalytic, electronic, and conductive properties due to the combination of porosity and organo‐inorganic nature. However, lab‐to‐fab transfer for 2D MOF layers faces the challenge of their scalability, limited by weak interactions between the organic and inorganic building blocks. Here, comparing three top‐down approaches to fabricate 2D MOF layers (sonication, freeze‐thaw, and mechanical exfoliation), The technological criteria have established for creation of the layers of the thickness up to 1 nm with a record aspect ratio up to 2*10^4:1. The freezing‐thaw and mechanical exfoliation are the most optimal approaches; wherein the rate and manufacturability of the mechanical exfoliation rivaling the greatest scalability of 2D MOF layers obtained by freezing‐thaw (21300:1 vs 1330:1 aspect ratio), leaving the sonication approach behind (with a record 900:1 aspect ratio) have discovered. The high quality 2D MOF layers with a record aspect ratio demonstrate unique optical sensitivity to solvents of a varied polarity, which opens the way to fabricate scalable and freestanding 2D MOF‐based atomically thin chemo‐optical sensors by industry‐oriented approach.

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Su, Alice, Petru Apostol, Jiande Wang, Alexandru Vlad und Mircea Dincă. „Electrochemical Capacitance Traces with Interlayer Spacing in Two‐dimensional Conductive Metal‐Organic Frameworks“. Angewandte Chemie International Edition, 28.02.2024. http://dx.doi.org/10.1002/anie.202402526.

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Electrically conductive metal‐organic frameworks (MOFs) are promising candidates for electrochemical capacitors (EC) due to their high specific surface areas and potential for redox activity. To maximize energy density, traditional inorganic pseudocapacitors have utilized faradaic processes in addition to double‐layer capacitance. Although conductive MOFs are usually comprised of redox active ligands which allow faradaic reactions upon electrochemical polarization, systematic studies providing deeper understanding of the charge storage processes and structure‐function relationships have been scarce. Here, we investigate the charge storage mechanisms of a series of triazatruxene‐based 2D layered conductive MOFs with variable alkyl functional groups, Ni3(HIR3‐TAT)2 (TAT = triazatruxene; R = H, Et, n‐Bu, n‐Pent). Functionalization of the triazatruxene core allows for systematic variation of structural parameters while maintaining in‐plane conjugation between ligands and metals. Specifically, R groups modulate interlayer spacing, which in turn shifts the charge storage mechanism from double‐layer capacitance towards pseudocapacitance, leading to an increase in molar specific capacitance from Ni3(HIH3‐TAT)2 to Ni3(HIBu3‐TAT)2. Partial exfoliation of Ni3(HIBu3‐TAT)2 renders redox active ligand moieties more accessible, and thus increases the dominance of faradaic processes. Our strategy of controlling charge storage mechanism through tuning the accessibility of redox‐active sites may motivate further design and engineering of electrode materials for EC.

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Su, Alice, Petru Apostol, Jiande Wang, Alexandru Vlad und Mircea Dincă. „Electrochemical Capacitance Traces with Interlayer Spacing in Two‐dimensional Conductive Metal‐Organic Frameworks“. Angewandte Chemie, 28.02.2024. http://dx.doi.org/10.1002/ange.202402526.

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Electrically conductive metal‐organic frameworks (MOFs) are promising candidates for electrochemical capacitors (EC) due to their high specific surface areas and potential for redox activity. To maximize energy density, traditional inorganic pseudocapacitors have utilized faradaic processes in addition to double‐layer capacitance. Although conductive MOFs are usually comprised of redox active ligands which allow faradaic reactions upon electrochemical polarization, systematic studies providing deeper understanding of the charge storage processes and structure‐function relationships have been scarce. Here, we investigate the charge storage mechanisms of a series of triazatruxene‐based 2D layered conductive MOFs with variable alkyl functional groups, Ni3(HIR3‐TAT)2 (TAT = triazatruxene; R = H, Et, n‐Bu, n‐Pent). Functionalization of the triazatruxene core allows for systematic variation of structural parameters while maintaining in‐plane conjugation between ligands and metals. Specifically, R groups modulate interlayer spacing, which in turn shifts the charge storage mechanism from double‐layer capacitance towards pseudocapacitance, leading to an increase in molar specific capacitance from Ni3(HIH3‐TAT)2 to Ni3(HIBu3‐TAT)2. Partial exfoliation of Ni3(HIBu3‐TAT)2 renders redox active ligand moieties more accessible, and thus increases the dominance of faradaic processes. Our strategy of controlling charge storage mechanism through tuning the accessibility of redox‐active sites may motivate further design and engineering of electrode materials for EC.

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Shang, Shengcong, Changsheng Du, Youxing Liu, Minghui Liu, Xinyu Wang, Wenqiang Gao, Ye Zou, Jichen Dong, Yunqi Liu und Jianyi Chen. „A one-dimensional conductive metal-organic framework with extended π-d conjugated nanoribbon layers“. Nature Communications 13, Nr. 1 (09.12.2022). http://dx.doi.org/10.1038/s41467-022-35315-0.

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AbstractConductive metal-organic frameworks (MOFs) have performed well in the fields of energy and catalysis, among which two-dimensional (2D) and three-dimensional (3D) MOFs are well-known. Here, we have synthesized a one-dimensional (1D) conductive metal-organic framework (MOF) in which hexacoordinated 1,5-Diamino-4,8-dihydroxy-9,10-anthraceneedione (DDA) ligands are connected by double Cu ions, resulting in nanoribbon layers with 1D π-d conjugated nanoribbon plane and out-of-plane π-π stacking, which facilitates charge transport along two dimensions. The DDA-Cu as a highly conductive n-type MOF has high crystalline quality with a conductivity of ~ 9.4 S·m−1, which is at least two orders of magnitude higher than that of conventional 1D MOFs. Its electrical band gap (Eg) and exciton binding energy (Eb) are approximately 0.49 eV and 0.3 eV, respectively. When utilized as electrode material in a supercapacitor, the DDA-Cu exhibits good charge storage capacity and cycle stability. Meanwhile, as thse active semiconductor layer, it successfully simulates the artificial visual perception system with excellent bending resistance and air stability as a MOF-based flexible optoelectronic synaptic case. The controllable preparation of high-quality 1D DDA-Cu MOF may enable new architectural designs and various applications in the future.

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Ma, Zhi-Zhou, Qiao-Hong Li, Zirui Wang, Zhi-Gang Gu und Jian Zhang. „Electrically regulating nonlinear optical limiting of metal-organic framework film“. Nature Communications 13, Nr. 1 (26.10.2022). http://dx.doi.org/10.1038/s41467-022-34139-2.

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AbstractRegulating nonlinear optical (NLO) property of metal−organic frameworks (MOFs) is of pronounced significance for their scientific research and practical application, but the regulation through external stimuli is still a challenging task. Here we prepare and electrically control the nonlinear optical regulation of conductive MOFs Cu-HHTP films with [001]- (Cu-HHTP[001]) and [100]-orientations (Cu-HHTP[100]). Z-scan results show that the nonlinear absorption coefficient (β) of Cu-HHTP[001] film (7.60 × 10−6 m/W) is much higher than that of Cu-HHTP[100] film (0.84 × 10−6 m/W) at 0 V and the β of Cu-HHTP[001] and Cu-HHTP[100] films gradually increase to 3.84 × 10−5 and 1.71 × 10−6 m/W at 10 V by increasing the applied voltage, respectively. Due to 2D Cu-HHTP having anisotropy of charge transfer in different orientations, the NLO of MOFs film can be dependent on their growth orientations and improved by tuning the electrical field. This study provides more avenues for the regulation and NLO applications of MOFs.

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Sirijaraensre, Jakkapan. „Sensing properties of 2D conductive M3(HITP)2 MOFs toward SO2 gas: a theoretical study“. Chemical Papers, 17.06.2023. http://dx.doi.org/10.1007/s11696-023-02921-1.

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Apostol, Petru, Sai Manoj Gali, Alice Su, Da Tie, Yan Zhang, Shubhadeep Pal, Xiaodong Lin et al. „Controlling Charge Transport in 2D Conductive MOFs─The Role of Nitrogen-Rich Ligands and Chemical Functionality“. Journal of the American Chemical Society, 03.11.2023. http://dx.doi.org/10.1021/jacs.3c07503.

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46

Liu, Limei, Yi Zhang, Yongzhen Song, Yijing Gu, Huan Pang und Rongmei Zhu. „Successful In Situ Growth of Conductive MOFs on 2D Cobalt-Based Compounds and Their Electrochemical Performance“. Inorganic Chemistry, 21.05.2024. http://dx.doi.org/10.1021/acs.inorgchem.4c01168.

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Yang, Luming, und Mircea Dincă. „Redox ladder of Ni3 complexes with closed‐shell, mono‐, and diradical triphenylene units: molecular models for conductive 2D MOFs“. Angewandte Chemie, 02.09.2021. http://dx.doi.org/10.1002/ange.202109304.

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Yang, Luming, und Mircea Dincă. „Redox ladder of Ni3 complexes with closed‐shell, mono‐, and diradical triphenylene units: molecular models for conductive 2D MOFs“. Angewandte Chemie International Edition, 02.09.2021. http://dx.doi.org/10.1002/anie.202109304.

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Li, Kuncai, Jing Wang und Hong Wang. „Recent Advance of 2D Conductive Metal-Organic Framework in Thermoelectrics“. Journal of Materials Chemistry A, 2024. http://dx.doi.org/10.1039/d4ta01820f.

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Conductive metal-organic frameworks (c-MOFs) are promising thermoelectric (TE) materials due to their low thermal conductivity and tunable electronic properties. Theoretical results show that two dimensional semiconuctors have natural advantages in...

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Jastrzembski, Kamil, Yingying Zhang, Yang Lu, Lukas Sporrer, Darius Pohl, Bernd Rellinghaus, Albrecht L. Waentig et al. „Tunable Crystallinity and Electron Conduction in Wavy 2D Conjugated Metal–Organic Frameworks via Halogen Substitution“. Small, 11.12.2023. http://dx.doi.org/10.1002/smll.202306732.

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AbstractCurrently, most reported 2D conjugated metal–organic frameworks (2D c‐MOFs) are based on planar polycyclic aromatic hydrocarbons (PAHs) with symmetrical functional groups, limiting the possibility of introducing additional substituents to fine‐tune the crystallinity and electrical properties. Herein, a novel class of wavy 2D c‐MOFs with highly substituted, core‐twisted hexahydroxy‐hexa‐cata‐benzocoronenes (HH‐cHBCs) as ligands is reported. By tailoring the substitution of the c‐HBC ligands with electron‐withdrawing groups (EWGs), such as fluorine, chlorine, and bromine, it is demonstrated that the crystallinity and electrical conductivity at the molecular level can be tuned. The theoretical calculations demonstrate that F‐substitution leads to a more reversible coordination bonding between HH‐cHBCs and copper metal center, due to smaller atomic size and stronger electron‐withdrawing effect. As a result, the achieved F‐substituted 2D c‐MOF exhibits superior crystallinity, comprising ribbon‐like single crystals up to tens of micrometers in length. Moreover, the F‐substituted 2D c‐MOF displays higher electrical conductivity (two orders of magnitude) and higher charge carrier mobility (almost three times) than the Cl‐substituted one. This work provides a new molecular design strategy for the development of wavy 2D c‐MOFs and opens a new route for tailoring the coordination reversibility by ligand substitution toward increased crystallinity and superior electric conductivity.

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