Review
Chemistry, Multidisciplinary
Yong-Sheng Wei, Christopher W. Ashling, Teerat Watcharatpong, Zeyu Fan, Satoshi Horike
Summary: Glassy states of network-forming coordination polymers and metal-organic frameworks represent a novel category of amorphous materials with diverse applications. Extensive studies have revealed the wide range of utility in gas permeability, conductivity, optics, and catalysis of these glasses. Additionally, their inherent properties and phase transformation capability allow for various morphological architectures.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wentao Xu, Nikita Hanikel, Kirill A. Lomachenko, Cesare Atzori, Alicia Lund, Hao Lyu, Zihui Zhou, C. Austen Angell, Omar M. Yaghi
Summary: We developed a synthetic strategy to link Ti-oxo clusters into MOF glasses using carboxylate linkage, resulting in high porosity. A new series of MOF glasses were fabricated by evaporating a solution containing Ti-oxo clusters, linkers, and m-cresol. The formation of carboxylate linkages was confirmed by FT-IR spectroscopy, and the structural integrity of Ti-oxo clusters was demonstrated by XANES and O-17 MAS NMR. After ligand exchange and activation, the Ti-Fum MOF glass exhibited a significantly higher BET surface area compared to previously reported phenolate-linked MOF glasses.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Chinmoy Das, Taichi Nishiguchi, Zeyu Fan, Satoshi Horike
Summary: This study investigated the mechanism of crystal melting and crystallization behavior of a two-dimensional coordination polymer during heating-cooling processes. The results showed that the coordination bond networks were partially retained in the melt state and the melt had a significantly lower viscosity compared to other samples. Rheological studies provided insights into the fast relaxation dynamics of the recrystallization process.
Article
Chemistry, Multidisciplinary
Rijia Lin, Xuemei Li, Andraz Krajnc, Zhiheng Li, Mengran Li, Wupeng Wang, Linzhou Zhuang, Simon Smart, Zhonghua Zhu, Dominique Appadoo, Jeffrey R. Harmer, Zhiliang Wang, Ana Guilherme Buzanich, Sebastian Beyer, Lianzhou Wang, Gregor Mali, Thomas D. Bennett, Vicki Chen, Jingwei Hou
Summary: The research introduces a novel method to fabricate a bimetallic MOF glass, demonstrating significantly enhanced catalytic performance by incorporating Fe nodes into the Co-based framework through a melt-quenching process. The technique, combined with mechanochemical synthesis, provides significant opportunities for catalytic device assembly on flexible substrates.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Luis Leon-Alcaide, Rasmus S. Christensen, David A. Keen, Jose L. Jorda, Isaac Brotons-Alcazar, Alicia Forment-Aliaga, Guillermo Minguez Espallargas
Summary: We describe the synthesis, phase transformations, and melting properties of the first meltable iron-based zeolitic imidazolate framework (ZIF), known as MUV-24. It is obtained through thermal treatment of [Fe3(im)6(Him)2], resulting in the formation of Fe(im)2. Upon further heating, different crystalline phase transformations are observed, until the material melts at 482 degrees C. Cooling of the liquid phase leads to the formation of the first Fe-metal-organic framework glass.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Shuyang Yao, Wei-Hui Fang, Yayong Sun, San-Tai Wang, Jian Zhang
Summary: This study introduces a novel supramolecular nanocage structure assembled from aluminum molecular rings, exhibiting superior iodine adsorption behavior. Single-crystal X-ray diffraction reveals the binding sites of molecular I-2 within the cages. The resulting adsorbent demonstrates a high iodine vapor saturation uptake capacity and can be recycled for further use.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Review
Chemistry, Multidisciplinary
Satoshi Horike, Nattapol Ma, Zeyu Fan, Soracha Kosasang, Morten M. Smedskjaer
Summary: The melting and glassy states of coordination polymers/metal-organic frameworks have attracted attention as a new class of amorphous materials with potential applications. The challenge in this field lies in developing design principles, achieving corresponding functions of mass transport and conversion, and integrating devices with tunable mechanical properties.
Article
Chemistry, Physical
Marco Bosi, Julian Fischer, Philipp Maass
Summary: A major challenge in modeling ionically conducting glasses is to understand how different chemical compositions and structures affect ionic transport quantities. Theoretical approaches have been developed to explain the variations of both network former unit concentrations and activation energies with glass composition, showing good agreement with experimental data for alkali borophosphate glasses.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Materials Science, Ceramics
Ting Zhang, Zhilin Long, Li Peng, Zhuang Li
Summary: In this paper, a convolutional neural network (CNN) model was used to investigate the glass forming ability (GFA) of bulk metallic glasses (BMGs). By training and testing with a large number of alloy compositions, the study shows that machine learning methods have great potential in guiding the design of new BMG materials.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2022)
Article
Chemistry, Multidisciplinary
Ashleigh M. Chester, Celia Castillo-Blas, Lothar Wondraczek, David A. Keen, Thomas D. Bennett
Summary: This study proposes the combination of MOFs with inorganic glasses to create novel composite materials, aiming to improve the processability issues and mechanical performance of MOFs. The materials are classified as crystalline MOF-glass composites and blends, with the goal of retaining the beneficial properties of both components.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Physical
Yangyang Han, Junbo Wang, Luying Song, Yuanjing Zheng, Youyong Li, Haiping Lin, Qing Li, Lifeng Chi
Summary: The research shows that shorter molecules tend to bond with extracted metal adatoms, forming metal-organic hybrids, while longer molecules prefer bonding with lattice metal atoms.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Materials Science, Ceramics
Florian Calzavara, Mathieu Allix, Marc Dussauze, Veronique Jubera, Marcelo Nalin, Thierry Cardinal, Evelyne Fargin
Summary: Researchers explored glass forming regions in the system GaO3/2 - GeO2 - LaO3/2 - BaO using aerodynamic levitation coupled with laser heating synthesis technique, and established structure-property relationships between the thermal and optical properties of resulting glass. They found that in GeO2-rich compositions, depolymerization of the glass network occurs due to the excess of positive charges.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2021)
Article
Chemistry, Physical
Nicolas Castel, Francois-Xavier Coudert
Summary: In this study, we extensively investigated the computation of finite temperature mechanical properties of ZIF-4 in both crystal and glass phases using various glass models. We critically assessed computational methodologies, including ab initio molecular dynamics, reactive force fields, and classical force fields. The results showed that the ZIF-4 glasses have a larger bulk modulus than the crystal, and the relationship between density and bulk modulus was confirmed for ZIF glasses, emphasizing the importance of obtaining accurate density models for predicting physical properties.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Nattapol Ma, Nao Horike, Loris Lombardo, Soracha Kosasang, Kotoha Kageyama, Chonwarin Thanaphatkosol, Kanokwan Kongpatpanich, Ken-ichi Otake, Satoshi Horike
Summary: By forming a binary CsHSO4-coordination polymer glass system, the superprotonic conductivity of CsHSO4 can be preserved below its transition temperature, resulting in significantly improved proton conductivity and processability compared to traditional CsHSO4. The method also enables the preparation of a thin-film proton conductor with low resistivity and high transparency. Solid-state NMR and X-ray pair distribution functions provide insights into the mechanism behind the preserved conductivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Biochemistry & Molecular Biology
Cristina del Mar Garcia Martin, Jose Ignacio Hernandez Garcia, Sebastian Bonardd, David Diaz Diaz
Summary: Carbon-carbon (C-C) bond formation is a vital reaction in organic synthesis, and there has been increasing interest in developing catalytic processes for C-C bond formation using renewable resources. Lignin, as a biopolymer-based material, has shown potential as a catalyst in various C-C formation reactions due to its heterogeneous nature, easy preparation, low cost, and the ability to recover and reuse the catalyst. This review highlights the successful applications of lignin-based catalysts in condensations, Michael additions of indoles, and Pd-mediated cross-coupling reactions.
Article
Chemistry, Multidisciplinary
Javier Troyano, Shuhei Furukawa, Satoshi Horike
Summary: By combining two complementary chemical moieties, a robust water-soluble cuboctahedral MOP with high solubility and stability in water was synthesized, demonstrating high potential for flexible porous building units. Furthermore, postsynthetic acid treatment can lead to a porous cage with increased gas uptake capacity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Ziqian Xue, Jia-Jia Zheng, Yusuke Nishiyama, Ming-Shui Yao, Yoshitaka Aoyama, Zeyu Fan, Ping Wang, Takashi Kajiwara, Yoshiki Kubota, Satoshi Horike, Ken-ichi Otake, Susumu Kitagawa
Summary: By manipulating the coordination geometries of metal centers, new porous coordination polymers (PCPs) with tunable structure and conductivity have been successfully achieved. These PCPs exhibit varying pore structures and conductivities, enabling modulated selectivity and sensitivity in gas sensing.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Soren S. Sorensen, Xiangting Ren, Tao Du, Ayoub Traverson, Shibo Xi, Lars R. Jensen, Mathieu Bauchy, Satoshi Horike, John Wang, Morten M. Smedskjaer
Summary: This work demonstrates that water can depolymerize polyhedra with labile metal-ligand bonds in a cobalt-based coordination network, resulting in nonstoichiometric glasses. The addition of water molecules promotes the breakage of network bonds and coordination number changes, thereby lowering melting and glass transition temperatures. These structural changes alter the physical and chemical properties of the glass, similar to the concept of modifiers in oxides. This approach can be extended to other transition metal-based coordination networks, enabling diversification of hybrid glass chemistry.
Article
Chemistry, Physical
Zeyu Fan, Yong-Sheng Wei, Hiroyasu Tabe, Tomotaka Nakatani, Chinmoy Das, Hiroki Yamada, Satoshi Horike
Summary: We propose a new approach to create porous glassy states in coordinationpolymer (CP) and metal-organic framework (MOF) by ball milling two dense 1D crystal structures, enabling selective gas sorption and reversible photochromism.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Haruki Sato, Koichiro Miyanishi, Makoto Negoro, Akinori Kagawa, Yusuke Nishiyama, Satoshi Horike, Koichi Nakamura, Munehiro Inukai
Summary: This study demonstrates the hyperpolarization of biomolecules in eutectic crystals using photoexcited triplet electrons at room temperature. The eutectic crystals, composed of benzoic acid doped with the polarization source and analyte domains, were prepared using a melting-quenching process. Solid-state NMR analysis elucidates spin diffusion between the benzoic acid and analyte domain, indicating the transfer of hyperpolarization from the benzoic acid domain to the analyte domain.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Zaoming Wang, Aydin Ozcan, Gavin. A. Craig, Frederik Haase, Takuma Aoyama, Daria Poloneeva, Keiji Horio, Masakazu Higuchi, Ming-Shui Yao, Cara. M. Doherty, Guillaume Maurin, Kenji Urayama, Anastasiya Bavykina, Satoshi Horike, Jorge Gascon, Rocio Semino, Shuhei Furukawa
Summary: A new concept of pore-networked gels is demonstrated by trapping the solvent phase with molecular networks to achieve accessible microporosity. These gels show enhanced CO2 capacities and improved mechanical properties and low volatility, making them potentially useful in gas adsorption and separation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Nattapol Ma, Sarawoot Impeng, Sareeya Bureekaew, Naoki Morozumi, Masa-aki Haga, Satoshi Horike
Summary: Scientists have successfully controlled the anhydrous proton conductivity in a transparent coordination polymer material through photoexcitation. They achieved reversible changes in proton conductivity by modulating light intensity and ambient temperature, providing total control of the conductivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Thanakorn Tiyawarakul, Thidarat Imyen, Kanokwan Kongpatpanich, Teerat Watcharatpong, Satoshi Horike
Summary: In this study, a method for macroscopic shaping of 1D coordination polymer was reported to overcome the difficulties in processing and recovery of catalytic materials in powder form. Glassy ZnPBIm monoliths of different shapes and sizes were prepared via a melt-quench process, and showed high catalytic activity and recyclability in the esterification reaction.
Article
Chemistry, Multidisciplinary
Siquan Zhang, Loris Lombardo, Masahiko Tsujimoto, Zeyu Fan, Ellan K. Berdichevsky, Yong-Sheng Wei, Kotoha Kageyama, Yusuke Nishiyama, Satoshi Horike
Summary: In this study, a environmentally friendly method for synthesizing crystalline COFs from CO2 molecules as a precursor was proposed. The COFs showed high stability and a large surface area, and remained stable under strong acid, base, and high temperature conditions. The hydrophobicity and proton conductivity of the COFs could be modulated through post-modification.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Hitoshi Izu, Hiroyasu Tabe, Yuji Namiki, Hiroki Yamada, Satoshi Horike
Summary: A transparent and grain boundary-free coordination polymer glass membrane immobilizing metalloporphyrins was studied as a heterogeneous photocatalyst for carbon dioxide reduction under visible-light irradiation. The photocatalytic activity of the membrane was proportional to its thickness, indicating that the metalloporphyrins in the subsurface of the membrane were photoexcited and contributed to the reactions. Transparent and grain boundary-free substrates are essential for efficient photoirradiation reactions without interference from light scattering and absorption.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Thi Ha My Pham, Tzu-Hsien Shen, Youngdon Ko, Liping Zhong, Loris Lombardo, Wen Luo, Satoshi Horike, Vasiliki Tileli, Andreas Zu''ttel
Summary: Ni- and Co-based catalysts with added Fe demonstrate promising activity in the oxygen evolution reaction (OER) during alkaline water electrolysis, with the presence of Fe in a certain quantity being crucial for their enhanced performance. The mechanism of Fe incorporation into a Co-based host was investigated, and the findings provide a comprehensive understanding of the role of Fe in Co-based electrocatalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Yong-Sheng Wei, Christopher W. Ashling, Teerat Watcharatpong, Zeyu Fan, Satoshi Horike
Summary: Glassy states of network-forming coordination polymers and metal-organic frameworks represent a novel category of amorphous materials with diverse applications. Extensive studies have revealed the wide range of utility in gas permeability, conductivity, optics, and catalysis of these glasses. Additionally, their inherent properties and phase transformation capability allow for various morphological architectures.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zeyu Fan, Yong-Sheng Wei, Chinmoy Das, Kazuyoshi Kanamori, Hiroki Yamada, Koji Ohara, Satoshi Horike
Summary: In this study, dicarboxylate-based coordination polymer glasses were formed directly through thermal dehydration. The rearrangement of coordination networks caused by dehydration was monitored using various characterization techniques. The microporosity and mechanical properties of these glasses were also investigated. Furthermore, a series of dicarboxylate-bridged networked glasses with tunable porosity and mechanical properties were obtained through the dehydration of hydrated coordination polymer crystals.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Chonwarin Thanaphatkosol, Nattapol Ma, Kotoha Kageyama, Teerat Watcharatpong, Thanakorn Tiyawarakul, Kanokwan Kongpatpanich, Satoshi Horike
Summary: Reversible solid-to-liquid phase transition allows for the formation of homogeneous mixed-glasses in coordination polymer glasses from two distinct parent compounds. The resulting mixed glasses exhibit composition-dependent glass transition temperatures and unique viscoelastic behavior. Non-linear mixed glass former effect and controllable anhydrous H+ conductivities are also demonstrated.
CHEMICAL COMMUNICATIONS
(2022)
