Article
Chemistry, Multidisciplinary
Jianli Wang, Yifan Mao, Runze Zhang, Yanli Zeng, Changsheng Li, Bingjie Zhang, Jianhui Zhu, Jiawen Ji, Desheng Liu, Rumin Gao, Yongqiang Ma
Summary: This study presents a universal scheme for synthesizing core-shell hybrids (MOF@HOF) by using stable HOFs and surface-functionalized MOFs. The newly synthesized NH2-UiO-66@DAT-HOF core-shell nanostructure exhibits excellent stability and superb photocatalytic performance, with an apparent reaction rate constant up to 60.7 and 7.6 times higher than its parent materials NH2-UiO-66 and DAT-HOF for tetracycline degradation. This enhancement is attributed to the broader visible-light utilization range and efficient charge carrier separation supported by the S-scheme heterojunction. Furthermore, the photocatalytic efficiency of the core-shell nanostructure remains high after several-cycle applications.
Article
Chemistry, Physical
Mohammad Shahinur Rahaman, Sarttrawut Tulaphol, Kyle Mills, Ashten Molley, Md Anwar Hossain, Shashi Lalvani, Thana Maihom, Mark Crocker, Noppadon Sathitsuksanoh
Summary: Lactic acid is a renewable and versatile chemical derived from biomass, and the development of water-tolerant acid catalysts is crucial for its production. The study demonstrates that the MIL-101(Al)-NH2 metal-organic framework is an efficient and selective solid Lewis acid catalyst for dihydroxyacetone isomerization to lactic acid, showing high selectivity and stability.
Article
Chemistry, Multidisciplinary
Xiwei Han, Xiaoxian Yang, Chuan Yu, Shuyan Lu, Ehsan Sadeghi Pouya, Peng Bai, Jiafei Lyu, Xianghai Guo
Summary: The modification of metal-organic frameworks by functionalizing ligands has been investigated in this study, leading to the construction of novel Zr-MOFs with improved adsorption properties towards CO2, CH4, N-2, and H-2 gases. Enhanced adsorption selectivity towards CO2/H-2 and improved high pressure H-2 adsorption were observed in the newly synthesized materials.
Article
Multidisciplinary Sciences
Yan Su, Ken-ichi Otake, Jia-Jia Zheng, Satoshi Horike, Susumu Kitagawa, Cheng Gu
Summary: Efficient separation of water isotopologues at room temperature has been achieved by constructing porous coordination polymers with flip-flop molecular motions to regulate the diffusion rates of water isotopologues. This method shows promise for high-performance vapor separation.
Article
Chemistry, Physical
Juan L. Obeso, J. Gabriel Flores, Catalina V. Flores, Reyna Rios-Escobedo, Julia Aguilar-Pliego, A. Ken Inge, Jose Antonio de los Reyes, Ricardo A. Peralta, Ilich A. Ibarra, Carolina Leyva
Summary: SU-101 was found to be an acid catalyst for the ring-opening alcoholysis of cyclohexene oxide, possessing open metal sites. It demonstrated high chemical stability, retaining its crystalline structure after the reaction. The conversion rates of cyclohexene to methanol, ethanol, and propanol were estimated to be 99.8%, 96.8%, and 14.3% at 40 degrees C, respectively. Moreover, SU-101 exhibited excellent catalytic cyclability, maintaining its activity after five cycles.
Review
Chemistry, Multidisciplinary
Haoxin Mai, Tu C. Le, Dehong Chen, David A. Winkler, Rachel A. Caruso
Summary: This article reviews the role of machine learning methods in clean energy applications, specifically in the design, discovery, and synthesis optimization of adsorbent materials. Through case studies, it demonstrates the importance of these methods in accelerating the development of high-performance adsorbent materials.
Article
Chemistry, Multidisciplinary
Long Jiao, Juntong Zhu, Yan Zhang, Weijie Yang, Siyuan Zhou, Aowen Li, Chenfan Xie, Xusheng Zheng, Wu Zhou, Shu-Hong Yu, Hai-Long Jiang
Summary: Through the direct pyrolysis of MOFs assembled with Fe and Ni-doped ZnO nanoparticles, a novel Fe-1-Ni-1-N-C catalyst with neighboring Fe and Ni single-atom pairs on nitrogen-doped carbon support has been precisely constructed. The synergism of neighboring Fe and Ni single-atom pairs significantly boosts the electrocatalytic reduction of CO2, surpassing catalysts with separate Fe or Ni single atoms. The study reveals the importance of the communicative effect between adjacent single atoms for improved catalysis in single-atom catalysts containing multiple metal species.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Mohammad Shahinur Rahaman, Sarttrawut Tulaphol, Anwar Hossain, Jacek B. Jasinski, Shashi B. Lalvani, Mark Crocker, Thana Maihom, Noppadon Sathitsuksanoh
Summary: Aluminum-containing metal-organic frameworks (Al-MOFs) show activity, selectivity, stability, and reusability for glucose isomerization in ethanol. Al-MOFs achieved high fructose selectivity at high glucose conversion, and the catalyst is stable and can be reused at least four times.
Article
Chemistry, Multidisciplinary
Yan Yue, Peiyu Cai, Xiaoyi Xu, Hanying Li, Hongzheng Chen, Hong-Cai Zhou, Ning Huang
Summary: This study demonstrates the potential of metallophthalocyanine-based conductive frameworks in advanced stand-off chemical sensors, showing high electrical conductivity and sensitivity in detecting low-concentration gases. The fabrication of thin films with different thicknesses also highlights the general strategy of tailor-made molecular design for developing sensitive and stable chemical sensors.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Inorganic & Nuclear
Zhehao Huang, Erik Svensson Grape, Jian Li, A. Ken Inge, Xiaodong Zou
Summary: Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) are important classes of porous materials, whose structure determination is crucial for their applications. Three-dimensional electron diffraction (3DED) methods have advanced significantly for structure elucidation of nano- and submicro-sized crystals.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Olga Kataeva, Kirill Metlushka, Kamil Ivshin, Zilya Yamaleeva, Ruzal Zinnatullin, Kristina Nikitina, Elena Badeeva, Vera Khrizanforova, Yulia Budnikova, Marco Naumann, Christoph Wellm, Alexey Alfonsov, Vladislav Kataev, Bernd Buechner, Martin Knupfer
Summary: The structures and properties of mononuclear and polymeric Co(ii) complexes formed by enantiopure and racemic N-thiophosphorylated thioureas with cobalt were studied in detail, and various analytical methods were used for characterization.
Article
Chemistry, Inorganic & Nuclear
De-Gang Ke, Sheng-Li Huang, Guo-Yu Yang
Summary: In this study, three polyoxometalate-based metal-organic frameworks were synthesized through the thermal reaction of pyridyl-Anderson polyoxometalate linker and lanthanide ions. These frameworks exhibited excellent photocatalytic sulfide oxidation performance with sulfoxide selectivity in the presence of [Ru(bpy)3]2+ photosensitizer.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Manik Shit, Satyajit Halder, Arka Dey, Basudeb Dutta, Anjana Chanthapally, Kuladip Jana, Chittaranjan Sinha
Summary: A novel 3D coordination framework material with semiconductor ability and excellent photoconductivity has been studied. The material shows significant anticancer activity against MDA-MB-231 cells. Therefore, it has important implications for the sustainable development goals in the fields of energy and health.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Analytical
Huijie Xu, Junli Guo, Junjian Zhao, Zhida Gao, Yan-Yan Song
Summary: In this study, an enantioselective artificial architecture was constructed on TiO2 nanochannels, using homochiral Ti-based metal-organic frameworks (MOFs) as the skeleton, Fe(III) as peroxidase-mimicking centers, and L-tartaric acid (TA) as a chiral recognition selector. The selective recognition of cystine enantiomers was achieved through hydrogen bonds formed between chiral cystine and the host, and the change in peroxidase-like activity of the nanochannels was monitored through ionic current signatures.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Zachary L. Magnuson, Qigan Cheng, Weijie Zhang, Yu-Sheng Chen, Lukasz Wojtas, Ayman Nafady, Abdullah M. Al-Enizi, Randy W. Larsen, X. Peter Zhang, Shengqian Ma
Summary: This study successfully synthesized two new metal-metalloporphyrin frameworks (MMPF-12 and MMPF-13) via solvothermal conditions, showing unique structures with either fully or partially metalated ligands, as well as selective adsorption of CO2 and catalytic activity towards CO2 cycloaddition. The enhanced catalytic activity of ligand-metalated MMPF-12 compared to MMPF-13 is likely attributed to the presence of trimer Mn clusters in its structure.
CRYSTAL GROWTH & DESIGN
(2021)
Article
Chemistry, Multidisciplinary
Wei Zheng, Kosuke Oki, Ranajit Saha, Yuh Hijikata, Eiji Yashima, Tomoyuki Ikai
Summary: Defect-free one-handed contracted helical tubular ladder polymers with a pi-electron-rich cylindrical helical cavity were synthesized and exhibited high enantioseparation abilities. The formation of the pi-electron-rich cylindrical helical cavity is key to the highly-enantioseparation ability. Molecular dynamics simulations suggested that chiral aromatics can be encapsulated by specific pi-pi and/or hydrophobic interactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Till J. B. Zaehringer, Julian A. Moghtader, Maria-Sophie Bertrams, Bibhisan Roy, Masanori Uji, Nobuhiro Yanai, Christoph Kerzig
Summary: To drive energy-demanding photoreactions under mild conditions, low-energy visible light can be converted to high-energy singlet states through triplet-triplet annihilation upconversion (TTA-UC). A new annihilator with a maximum emission wavelength in the UVB region, when combined with an organic sensitizer, enables blue-to-UVB upconversion. This study demonstrates a novel blue light-driven substrate or solvent activation strategy through UC-FRET reactions and paves the way for more sustainable light-to-chemical energy conversion systems.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Geoffrey Roberts, Jonathan Haslam, Satoshi Maeda
Summary: In this study, a workflow employing the AFIR method was used to investigate the self-assembly process of the SIFSIX-3-Zn MOF. Multiple competing pathways involving interconvertible intermediates were identified, providing a plausible explanation for the stochastic multistage processes believed to be key in MOF formation. This work represents the first application of an automated reaction mechanism discovery method to a MOF system.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Koki Nishimura, Reiya Yabuki, Tomoyuki Hamachi, Nobuo Kimizuka, Kenichiro Tateishi, Tomohiro Uesaka, Nobuhiro Yanai
Summary: By introducing a flexible linker into the hybrid system of porphyrin and TEMPO, efficient and long-lasting dynamic electron polarization (DEP) is achieved. The structural flexibility of the linker switches the interaction between the radical and the triplet, promoting the DEP process by bringing them into close proximity and avoiding rapid decay due to strong interactions. As a result, the new hybridized system exhibits a larger and more than 10 μs lasting DEP compared to the unlinked system.
JOURNAL OF PHYSICAL CHEMISTRY B
(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, Multidisciplinary
Tomoyuki Ikai, Sayaka Miyoshi, Kosuke Oki, Ranajit Saha, Yuh Hijikata, Eiji Yashima
Summary: We report the synthesis and resolution of a fully p-conjugated helical ladder polymer with a rigid helical cavity, composed of achiral units. The isolated excess one-handed helical ladder polymer showed strong circular dichroism and thermal stability, maintaining its optical activity in solution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yuya Inaba, Jian Yang, Yu Kakibayashi, Tomoki Yoneda, Yuki Ide, Yuh Hijikata, Jenny Pirillo, Ranajit Saha, Jonathan L. Sessler, Yasuhide Inokuma
Summary: In this study, a calixpyrrole-based chiral macrocyclic system, calix[1]furan[1]pyrrole[1]thiophene (1), was synthesized from an oligoketone. The macrocycle adopts a partial cone conformation and undergoes racemization via ring inversion. N-methylation of the pyrrole moiety suppresses racemization and enables chiral resolution. Furthermore, this system can also serve as a precursor to yield various calix[n]furan[n]pyrrole[n]thiophene products (n = 2-4), including the largest calix[n]pyrrole-like species to be structurally characterized.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Mikhail Tsitsvero, Jenny Pirillo, Yuh Hijikata, Tamiki Komatsuzaki
Summary: Nuclear magnetic resonance (NMR) spectroscopy is a crucial technique in chemistry for obtaining accurate information about molecules. This study presents a machine learning (ML) method based on Gaussian process/deep kernel learning to predict, average, and analyze instantaneous chemical shifts of molecular conformations. The method was successfully applied to a trefoil knot molecule composed of 24 para-connected benzene rings.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Akito Fukui, Keigo Matsuyama, Hiroaki Onoe, Shun Itai, Hidekazu Ikeno, Shunsuke Hiraoka, Kousei Hiura, Yuh Hijikata, Jenny Pirillo, Takahiro Nagata, Kuniharu Takei, Takeshi Yoshimura, Norifumi Fujimura, Daisuke Kiriya
Summary: In this paper, a selective DMF sensor using a molybdenum disulfide (MoS2) field-effect transistor (FET) is proposed. The sensor responds to DMF molecules but not to similar molecules of formamide, N,N-diethylformamide, and N,N-dimethylacetamide. The thin structure of MoS2-FET can be incorporated into a microfluidic chamber, which allows for real-time DMF monitoring by exchanging solutions subsequently. The designed device shows DMF monitoring in NaCl ionic solutions from 1 to 200 μL/mL. This work proposes the concept of selectively monitoring redox-inactive molecules based on the nonideal atomic affinity site on the surface of two-dimensional semiconductors.
Article
Chemistry, Multidisciplinary
Ryo Ohtani, Jianeng Xu, Junichi Yanagisawa, Yuudai Iwai, Takumi Ehara, Kiyoshi Miyata, Ken Onda, Jenny Pirillo, Yuh Hijikata, Tomoaki Hiraoka, Shinya Hayami, Benjamin Le Ouay, Masaaki Ohba
Summary: We synthesized an organic-inorganic hybrid material that undergoes drastic structural changes upon exposure to water vapor. The change in structure results in different photo-physical properties, with one form emitting near-infrared light and shifting to blue with increasing temperature, while the other form emits visible light and shifts to red.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Tomohiro Fukushima, Motoki Fukasawa, Kei Murakoshi
Summary: The oxygen evolution reaction (OER) is a crucial process for hydrogen production in water electrolysis. This study used a machine-learning-based approach to extract the reaction pathway from experimental data. Genetic algorithms were used to search for thermodynamic and kinetic parameters using the current-electrochemical potential relationship of the OER. Through the analysis of datasets, the energy state distributions of reaction intermediates were revealed, which can help in the design of catalysts for efficient hydrogen production.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Haruka Yoshino, Masaki Saigo, Kiyoshi Miyata, Ken Onda, Jenny Pirillo, Yuh Hijikata, Wataru Kosaka, Hitoshi Miyasaka
Summary: A luminescent three-dimensional coordination polymer (CP) of [Cd-II(pmd){Ag-I(CN)(2)}(2)] (1; pmd = pyrimidine) with two different coordination modes of Ag+ ions was synthesized. 1 exhibited thermochromic luminescence with positive thermal elongation of the Ag center dot center dot center dot Ag distance. Moreover, 1 showed a bright phosphorescence with the highest photoluminescence quantum yield (Phi(em)), approximately 60% at room temperature, among previously reported phosphorescent Ag-based CPs or metal-organic frameworks.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Tomohiro Fukushima, Soushi Yoshimitsu, Kei Murakoshi
Summary: The study demonstrates that modifications of the dynamic hydration structure can alter ion dynamics and conductivity. Vibrational strong coupling is shown to modify the friction experienced by hydrated ions and promote charge transport. This research reveals the potential role of polaritons in designing materials with enhanced ionic conduction.
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)
