Article
Multidisciplinary Sciences
Li-Hao Xu, Shen-Hui Li, Heng Mao, Yan Li, Ao-Shuai Zhang, Sen Wang, Wei-Min Liu, Jing Lv, Tao Wang, Wei-Wei Cai, Le Sang, Wen-Wen Xie, Chan Pei, Zheng-Zheng Li, Ying-Nan Feng, Zhi-Ping Zhao
Summary: This study presents a strategy to create highly flexible metal-organic framework nanosheet membranes for alcohol-water separation. The membranes exhibited ultrafast transport channels and achieved high flux and separation performance.
Article
Chemistry, Multidisciplinary
Caoling Li, Jian Shen, Kangbing Wu, Nianjun Yang
Summary: The properties and applications of metal-organic frameworks (MOFs) can be tuned by their metal centers and organic ligands. Specifically, 2D Cu-2MI exhibits strong adsorption energies and the biggest intrinsic rate constants towards analytes, enabling accurate and comparable monitoring in real samples.
Article
Chemistry, Multidisciplinary
Rajashree Newar, Naved Akhtar, Neha Antil, Ajay Kumar, Sakshi Shukla, Wahida Begum, Kuntal Manna
Summary: This study presents a strategy to develop eco-friendly asymmetric catalysts using naturally occurring amino acids and earth-abundant metals, resulting in highly active and enantioselective catalysts for hydrosilylation and hydroboration of carbonyl compounds by grafting amino acids within the pores of a metal-organic framework (MOF) and post-synthetic metalation with iron precursor. The MOF-Fe catalyst exhibited high turnover numbers and good recyclability, demonstrating higher activity and enantioselectivity compared to its homogeneous control catalyst due to the formation of robust single-site catalyst in the MOF through site-isolation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Inorganic & Nuclear
Chengfeng Zhu, Hongzhao Wang, Yongfei Mu, Ziwei Zhang, Lanjun Cheng, Tianfu Li, Yanming Fu, Xiang Wu, Yougui Li
Summary: The chiral metal-organic framework constructed from camphoric acid and a dipyridyl ligand has open chiral channels and multiple recognition sites, making it an efficient chiral solid adsorbent capable of separating racemic alcohols and epoxides with excellent enantioselectivities.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Arijit Halder, Ryan A. Klein, Sarah Shulda, Gavin A. McCarver, Philip A. Parilla, Hiroyasu Furukawa, Craig M. Brown, C. Michael McGuirk
Summary: Step-shaped adsorption-desorption of gaseous payloads by flexible metal-organic frameworks can facilitate the delivery of large usable capacities with reduced energetic penalties. The multivariate linker approach is a powerful tool for tuning the phase change behavior of flexible frameworks. In this work, a multivariate framework was developed with a considerably reduced threshold pressure and desirable adsorption-desorption profile for efficient storage and delivery of weakly physisorbing species.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jiahui Xian, Suisheng Li, Hui Su, Peisen Liao, Shihan Wang, Yawei Zhang, Wenqian Yang, Jun Yang, Yamei Sun, Yaling Jia, Qinglin Liu, Qinghua Liu, Guangqin Li
Summary: In this study, an innovative method for artificially synthesizing alpha-amino acids from nitric oxide (NO) was demonstrated. The process involved electrocatalytic reactions with alpha-keto acids using an atomically dispersed Fe supported on N-doped carbon matrix (AD-Fe/NC) catalyst. The conversion of nitrogen oxides into high-value products was achieved through a series of reactions, including the conversion of NO into hydroxylamine and subsequent nucleophilic attack on the alpha-keto acid. This research not only contributes to the artificial synthesis of amino acids but also promotes the development of near-zero-emission technologies for global environmental and economic advancement.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(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
Davide Balestri, Paolo P. Mazzeo, Roberto Perrone, Fabio Fornari, Federica Bianchi, Maria Careri, Alessia Bacchi, Paolo Pelagatti
Summary: Metal-organic frameworks (MOFs) offer the opportunity to confine guest molecules within their pores, with PUM168 being a Zn-based MOF capable of encapsulating a significant number of guest molecules, especially natural essential oil components. By utilizing single crystal X-ray diffraction, researchers were able to monitor the complex guest exchange process and study the structural evolution of DMF-to-guest replacement inside the MOF crystal. The correlation between supramolecular arrangement in the pores and selective guest release was investigated over time and temperature using static headspace GC-MS analysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Ping Wang, Ziqian Xue, Otake Ken-ichi, Susumu Kitagawa
Summary: In this study, a flexible porous coordination polymer (PCP) containing nitroxyl radicals was prepared to achieve controllable size-selective aerobic oxidation of alcohols by reversible switching between large- and contracted-pore configurations in response to solvent change.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Lun Shu, Yuan Peng, Rui Yao, Hongling Song, Chenyu Zhu, Weishen Yang
Summary: A facile strategy has been developed to construct defect-free and flexible metal-organic framework (MOF)-based membranes with high selectivity. The fabricated soft-solid MOF composite membranes showed excellent separation performance for H-2/CO2 separation. This study demonstrates the potential of MOF-based membranes in practical separation applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Applied
Zhuo Sun, Juan Lu, Xin Zhang, Xiangyu Shan, Qian Wu, Chao Li, Huiling Li, Shuning Yang, Li Tian
Summary: In this study, Zn-MOF electrospun nanofibres (Zn-MOF NFs), CdTe, and Au@Pt-rGo were used to construct a Ru(bpy)32+/tri-n-propylamine electrochemiluminescence (ECL) system, and a novel ECL sensor for the determination of fenpropathrin was developed for the first time. The Zn-MOF NFs with large surface area and pores could carry CdTe and Au@Pt-rGo, facilitating electron transfer and reducing electron transport paths, leading to enhanced luminescence. CdTe participated in the luminescence reaction and improved the system's sensitivity, while Au@Pt-rGo promoted electron transport. The constructed ECL sensor showed satisfactory results in weak alkaline solution, capable of detecting fenpropathrin in the range of 4 x 10- 11-4 x 10-6 M with a detection limit of 1.33 x 10-11 M (S/N = 3). It can be used for fenpropathrin detection in juice samples, providing a new approach for determining fenpropathrin.
Article
Chemistry, Multidisciplinary
Zhongyuan Zeng, Jian Wang, Shuang Zhao, Yuchan Zhang, Jingchuan Fan, Hui Wu, Jiajia Chen, Zaikuan Zhang, Zexuan Meng, Lu Yang, Renzhi Wang, Bo Zhang, Guixue Wang, Chen-Zhong Li, Guangchao Zang
Summary: A flexible H2O2 sensor has been constructed to monitor the dynamics of H2O2 in tumor cells and reveal the potential mechanism underlying the selective killing of tumor cells by ascorbic acid. The findings suggest that the oxidation product of ascorbic acid may be the substance that actually acts on tumor cells in tumor therapy.
Review
Chemistry, Analytical
Xu Xu, Muyao Ma, Tongxin Sun, Xin Zhao, Lei Zhang
Summary: Metal-organic frameworks (MOFs) have significant structural advantages and are applicable in various fields. They can encapsulate a variety of luminescent guest species, giving them a broader luminescent capability. This review systematically introduces the applications of various LG@MOF sensors in fluorescence detection of ions, biomarkers, pesticides, and preservatives, as well as the development of portable visual fluorescence sensing applications. The challenges and potential for future growth in these sectors are also briefly discussed.
Review
Chemistry, Multidisciplinary
Dongming Cai, Zhuxian Yang, Rui Tong, Haiming Huang, Chuankun Zhang, Yongde Xia
Summary: The fast development of Internet of Things and wearable electronics has created a demand for cost-effective and efficient electroactive materials for flexible energy storage devices. Binder-free nanostructured arrays have gained attention due to their ability to promote fast electron/ion transportation, withstand bending or twisting, and enhance the capacity of the whole device. The use of binder-free metal-organic framework (MOF) nanoarrays and MOF-derived nanoarrays with high surface area and unique porous structure has shown great potential in energy storage and has been extensively explored. This review compares and discusses the common substrates used for binder-free nanoarrays, analyzes the electrochemical performance of various MOF-based and MOF-derived nanoarrays, and examines their applications in flexible energy storage. The review also highlights key technical issues and future developments in this field.
Article
Chemistry, Multidisciplinary
Xiang He
Summary: Flexible bimetallic MOFs have been investigated for their dynamic behaviors and catalytic abilities through density functional theory calculations. Structural modulation of the MOFs can alter the catalytic performance and provide potential avenues for enhanced efficiency.
Article
Biochemistry & Molecular Biology
Saravanan Kandasamy, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, John M. Gardiner
Summary: 5-O-protected and 1,2-acetonide-protected D-glucurono-6,3-lactone furanosides were converted into novel furano-glucuronamides through treatment with ammonia. Different protection and deprotection routes led to primary gluconamide derivatives, while benzylations led to silyl migration, N-benzylation, or reclosure to lactone. The use of 5-O-PMB protection provided a method for obtaining fully protection-differentiated glucofuranamide. Crystal structures of fully protected glucurono-6,3-lactone lactone and glucuronamide derivatives were reported.
CARBOHYDRATE RESEARCH
(2023)
Article
Chemistry, Medicinal
Laura N. Jeffreys, Alison Ardrey, Taghreed A. Hafiz, Lauri-Anne Dyer, Ashley J. Warman, Nada Mosallam, Gemma L. Nixon, Nicholas E. Fisher, W. David Hong, Suet C. Leung, Ghaith Aljayyoussi, Jaclyn Bibby, Deepak V. Almeida, Paul J. Converse, Nader Fotouhi, Neil G. Berry, Eric L. Nuermberger, Anna M. Upton, Paul M. O'Neill, Stephen A. Ward, Giancarlo A. Biagini
Summary: This study successfully expressed Mycobacterium tuberculosis cytochrome bd oxidase and identified a series of inhibitors that can effectively suppress bacterial growth, suggesting their potential as antitubercular agents.
ACS INFECTIOUS DISEASES
(2023)
Article
Chemistry, Physical
Lin-jie Yang, Wenye Xuan, David Webster, Lethy Krishnan Jagadamma, Teng Li, David N. Miller, David B. Cordes, Alexandra M. Z. Slawin, Graham A. Turnbull, Ifor D. W. Samuel, Hsin-Yi Tiffany Chen, Philip Lightfoot, Matthew S. Dyer, Julia L. Payne
Summary: One of the advantages of organic-inorganic metal halides is their highly tuneable structures and properties, which are important for optimizing materials for photovoltaics and optoelectronic devices. In this study, bromine was included in a layered perovskite to induce a decrease in band gap and a structural transition. The inclusion of bromine also resulted in the formation of a new band in the electronic structure and a significant increase in mobility and/or carrier concentration. This work highlights the potential of molecular inclusion as a tool to tune the electronic properties of layered organic-inorganic perovskites.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Bogdana Borca, Tomasz Michnowicz, Fernando Aguilar-Galindo, Remi Petuya, Marcel Pristl, Verena Schendel, Ivan Pentegov, Ulrike Kraft, Hagen Klauk, Peter Wahl, Andres Arnau, Uta Schlickum
Summary: The changes in properties and preferential interactions based on subtle energetic differences are important for the functionalities of organic molecules in biological systems. The molecular adsorption and bonding to surfaces are determined by slightly energetically favored interactions, which define their properties in technological applications. In this study, the adsorption configurations of prochiral tetracenothiophene molecules on the Cu(111) surface are determined using Scanning Tunneling Microscopy and first-principles calculations. Interestingly, the adsorption sites are selected by chemically different moieties of the molecules based on the arrangement of atoms in the first and second surface layers. The thermal effects on the direct desulfurization reaction catalyzed by the Cu substrate are also investigated, resulting in covalently bound chiral configurations of the product.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Tao-Yuan Yu, Qian Niu, Yifa Chen, Meng Lu, Mi Zhang, Jing-Wen Shi, Jiang Liu, Yong Yan, Shun-Li Li, Ya-Qian Lan
Summary: A sevenfold interpenetrating 3D covalent organic framework (TPDT-COF) was synthesized and applied for selective photoisomerization and photocyclization of stilbene under mild conditions. By changing the gas atmosphere, cis-stilbene or phenanthrene can be formed with >99% selectivity. The study provides insights into the application of porous crystalline materials in selective photoisomerization and photocyclization.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Marita O'Sullivan, Jonathan Alaria, Matthew S. Dyer, John B. Claridge, Michael W. Gaultois, Matthew J. Rosseinsky
Summary: Epitaxial heterostructures composed of metal oxides offer a route to investigate emergent phenomena such as topological states and spin liquids. In this study, we report on the epitaxial growth, structural and electrical properties of metallic pyrochlore bismuth ruthenate heterostructures. Our findings indicate that Bi2Ru2O7 exhibits semimetallic behavior and strong electron-electron interactions. These results provide insights into the electronic structure and emergent topological properties of Bi2Ru2O7.
Article
Chemistry, Multidisciplinary
Luis Martinez-Crespo, Inigo J. Vitorica-Yrezabal, George F. S. Whitehead, Simon J. Webb
Summary: Relaying conformational change over several nanometers is crucial in allosterically regulated proteins. Scientists have successfully replicated this mechanism using nanometer-sized molecules that can reversibly switch between defined shapes in response to signaling molecules. The study demonstrated that a 1.8 nm long rigid rod molecule can serve as a switchable multi-squaramide hydrogen-bond relay, with each relay adopting different orientations based on proton signals and undergoing reversible changes. Additionally, a chemical fuel acted as a dissipative signal, causing the relay to return to its original orientation when consumed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Organic
Alexander C. Brannan, Elvie F. P. Beaumont, Nguyen Le Phuoc, George F. S. Whitehead, Mikko Linnolahti, Alexander S. Romanov
Summary: Organic TADF material 4BGIPN, based on benzoguanidine donor, shows impressive electronic properties and potential for the third generation of OLEDs. It emits yellow-green light with fast radiative rate and high photoluminescence quantum yield. With its stable highest occupied molecular orbital and lowest unoccupied molecular orbital, 4BGIPN is suitable for application as the electron transport layer or TADF class III emitter in OLEDs.
BEILSTEIN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Rajeh Alotaibi, Amy Booth, Edmund Little, Adam Brookfield, Amritroop Achari, Selena J. Lockyer, Grigore A. Timco, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, Nicholas F. Chilton, Rahul R. Nair, David Collison, Richard E. P. Winpenny
Summary: We synthesized and characterized a series of heterometallic rings using alkylammonium or imidazolium cations as templates. The structure of these rings can be controlled by the template and the coordination geometry preference of each metal, resulting in rings with eight, nine, ten, twelve, and fourteen metals. The compounds were analyzed using various techniques, including X-ray diffraction, elemental analysis, magnetometry, and EPR measurements. The magnetic measurements showed antiferromagnetic exchange coupling between the metal centers, while the EPR spectroscopy revealed different ground and excited states for different ring structures. These findings provide insights into the transferability of magnetic parameters among related compounds.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Organic
Nicolas Fantozzi, Remi Petuya, Alberto Insuasty, Germain Salvato Vallverdu, Emilie Genin, Didier Begue, Alexandre Martinez, Sandra Pinet, Isabelle Gosse
Summary: A fluorescent cage receptor that detects choline in pseudophysiological medium is discussed. The capsule forms a complex with choline in buffered medium, with an association constant greater than 9.9 x 104 M-1, and it exhibits selectivity towards acetylcholine.
Article
Chemistry, Organic
Nicolas Fantozzi, Remi Petuya, Alberto Insuasty, Germain Salvato Vallverdu, Emilie Genin, Didier Begue, Alexandre Martinez, Sandra Pinet, Isabelle Gosse
Summary: This article describes a fluorescent cage receptor that is able to detect choline in pseudophysiological medium. The receptor forms a complex with choline in buffered medium, with an association constant greater than 9.9 x 104 M-1, and shows selectivity towards acetylcholine.
Article
Materials Science, Multidisciplinary
Hong Cai, Ruiyong Chen, Mounib Bahri, Cara J. Hawkins, Manel Sonni, Luke M. Daniels, Jungwoo Lim, Jae A. Evans, Marco Zanella, Leanne A. H. Jones, Troy D. Manning, Tim D. Veal, Laurence J. Hardwick, Matthew S. Dyer, Nigel D. Browning, John B. Claridge, Matthew J. Rosseinsky
Summary: We successfully synthesized a new spinel-like oxyfluoride Li1.25Ni0.625Mn1.125O3F with significant cation disorder. Its crystal structure was confirmed by combined refinement of X-ray and neutron diffraction data. Li1.25Ni0.625Mn1.125O3F showed capacities of 225mAh/g and 285mAh/g at 25 and 40 degrees C, respectively, by intercalation of additional Li+ into the lattice. Compared to previously reported lithium transition metal disordered rocksalt or spinel-like oxyfluorides, Li1.25Ni0.625Mn1.125O3F exhibited significantly improved cycling stability with high structural integrity.
ACS MATERIALS LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Tom S. Bennett, Selina Nawaz, Selena J. Lockyer, Deepak Asthana, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, Grigore A. Timco, Neil A. Burton, Richard E. P. Winpenny, Eric J. L. McInnes
Summary: This study reports the synthesis and structural characterization of four [7]rotaxanes formed by coordinating hybrid inorganic-organic [2]rotaxanes to a central {Ni12} core. X-ray single crystal diffraction shows the formation of [7]rotaxanes with different conformations in the crystal. Small angle X-ray scattering and molecular dynamic simulations confirm the stability of the large molecules in solution and reveal different conformers than those found in the crystal. Pulsed EPR spectroscopy demonstrates a slight reduction in phase memory times for the {Cr7Ni} rings, which are proposed as qubits, in the presence of the {Ni12} cage.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Bono van IJzendoorn, Jessica B. M. Whittingham, George F. S. Whitehead, Nikolas Kaltsoyannis, Meera Mehta
Summary: In this study, the boron functionalized [P7] cluster was applied in organic transformations, including dearomatized reduction of pyridines and hydroboration of imines and nitriles, leading to the synthesis of amine compounds. The catalyst exhibited high stability and could be recycled multiple times without loss in performance. The mechanism of the pyridine reduction was investigated experimentally and computationally. This work demonstrates the potential of boron functionalized phosphorus Zintl clusters as transition metal-free catalysts for nitrogen-containing substrates.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Bono van IJzendoorn, Jessica B. M. Whittingham, George F. S. Whitehead, Nikolas Kaltsoyannis, Meera Mehta
Summary: This study demonstrates that boron functionalized phosphorus Zintl cluster can serve as a catalyst for the reduction of nitrogen containing substrates. The catalyst showed high stability and could be recycled multiple times without loss in performance.
DALTON TRANSACTIONS
(2023)
