Article
Chemistry, Physical
Qinlong Hong, Wenjing Wang, Shumei Chen, Ke Chen, Meng Liu, Hai-Xia Zhang, Jian Zhang
Summary: A novel microporous boron imidazolate framework (BIF-108-Zn) has been reported for efficient separation of ethylene and ethane by integrating organic ligands and extra-framework species as pore partition agents. The structure features high pore volume, reduced pore size, and functionalized pore surface for preferential binding of ethane. Dynamic breakthrough measurements show that BIF-108-Zn can produce polymer-grade ethylene with good regenerability and high stability.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Wen-Qi Tang, Ying-Jie Zhao, Ming Xu, Jin-Ya Xu, Sha-Sha Meng, Yun-Dong Yin, Qing-Hua Zhang, Lin Gu, Da-Huan Liu, Zhi-Yuan Gu
Summary: Control over the stacking modes of metal-organic framework (MOF) nanosheets can lead to excellent gas chromatographic separations. Different solvents can induce twisted stacking of nanosheets, while alkanes may result in untwisted stacking.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Philip M. Stanley, Johanna Haimerl, Christopher Thomas, Alexander Urstoeger, Michael Schuster, Natalia B. Shustova, Angela Casini, Bernhard Rieger, Julien Warnan, Roland A. Fischer
Summary: The co-immobilization of a CO2 reduction catalyst and a photosensitizer within metal-organic frameworks was studied, with specific host pore size affecting the spatial location of the catalyst and photosensitizer. This spatial arrangement influenced catalyst stability, electronic communication, and catalytic rates, providing insights for an optimized supramolecular layout.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Lixia Guo, Xue Han, Yujie Ma, Jiangnan Li, Wanpeng Lu, Weiyao Li, Daniel Lee, Ivan da Silva, Yongqiang Cheng, Svemir Rudic, Pascal Manuel, Mark D. Frogley, Anibal J. Ramirez-Cuesta, Martin Schroder, Sihai Yang
Summary: In this study, a systematic investigation of the adsorption mechanism of ammonia in MFM-300(Sc) was conducted using a combination of in situ neutron powder diffraction, inelastic neutron scattering, synchrotron infrared microspectroscopy, and solid-state Sc-45 NMR spectroscopy. The results revealed the formation of reversible host-guest supramolecular interactions, which directly explained the excellent reversibility observed in this material over 90 adsorption-desorption cycles.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Xi Chen, Sergei Sapchenko, Wanpeng Lu, Ming Li, Meng He, Yinlin Chen, Mark D. Frogley, Ivan da Silva, Sihai Yang, Martin Schroder
Summary: Metal-organic framework (MOF) materials have gained increasing interest in electronics due to their diverse structures, intrinsic porosity, and designable host-guest interactions. In this study, we investigated the dielectric properties of a series of robust materials, MFM-300(M) (M = Al, Sc, Cr, Fe, Ga, In), upon exposure to different guest molecules. We found that MFM-300(Fe) showed the highest increase in dielectric constant when adsorbing NH3, indicating its potential as a powerful dielectric-based sensor for NH3. Structural analysis and spectroscopy confirmed the electron delocalization induced by host-guest interactions between NH3 and the MOF host, resulting in structural polarization and a high dielectric constant.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jieyu Zheng, Larissa K. S. von Krbek, Tanya K. Ronson, Jonathan R. Nitschke
Summary: Spin-crossover (SCO) metal-organic cages have the potential to be used as magnetic sensors and switches. Variations in the donor strength of heterocyclic aldehyde subcomponents in imine-based ligands can tune the ligand field for a Fe-II center, resulting in diverse SCO behaviors in the cages. The tetrahedral SCO cage built from 1-methyl-1H-imidazole-2-carbaldehyde can encapsulate various guests and stabilize different cage spin states depending on guest size. The SCO tetrahedron also exhibits different affinities for guests in different spin states, which is attributed to subtle structural differences caused by the change in the metal center spin state.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Michelle Ernst, Ganna Gryn'ova
Summary: Metal-organic frameworks (MOF) and covalent organic frameworks (COFs) have potential as nanocarriers for targeted drug delivery. Noncovalent interactions between frameworks and drugs play a crucial role in drug uptake and release. This study demonstrates a good agreement between experimentally measured release metrics and in silico computed host-guest interaction energies for a range of drugs and frameworks. The findings suggest that framework functional groups significantly impact the strength of host-guest interactions and that a given framework can be an efficient delivery agent for various drugs beyond the typical ones.
HELVETICA CHIMICA ACTA
(2023)
Article
Engineering, Chemical
Shao-Min Wang, Fei Wang, Yong-Li Dong, Mohana Shivanna, Qiubing Dong, Xuan-Tong Mu, Jingui Duan, Qingyuan Yang, Michael J. Zaworotko, Qing-Yuan Yang
Summary: The research presents two interpenetrated diamondoid coordination networks capable of efficiently separating ethane from ethylene with high selectivity and uptake capacity. Experimental validation of the separation performance was conducted, and the mechanism was clarified through simulations and calculations. This demonstrates the significant potential of these materials as effective adsorbents for ethylene purification in practice.
SEPARATION AND PURIFICATION TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Na Cao, Honglei Wang, Yujie Ban, Yuecheng Wang, Kun Yang, Yingwu Zhou, Meng Zhao, Weiqiao Deng, Weishen Yang
Summary: By controlling the microenvironment and modifying hydrated MIL-53 with diversified terephthalic acid linkers, efficient capture of high-boiling-point furfural was achieved with high capture ratio and recovery rate.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Inorganic & Nuclear
Xi Yang, Di Yuan, Jinhong Hou, Adam C. Sedgwick, Suying Xu, Tony D. James, Leyu Wang
Summary: The field of supramolecular chemistry has rapidly expanded and become highly influential in various areas like biomedicine, energy materials, catalysis, and sensing. The combination of host/guest chemistry with functional inorganic nanoparticles has led to many new applications in drug delivery, bioimaging, and sensing. Recent progress in the development of organic/inorganic supramolecular nano-systems incorporating host/guest chemistry has been summarized, highlighting their applications in drug delivery, biological imaging, and sensing.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Multidisciplinary
Jun Zhang, Wataru Kosaka, Yasutaka Kitagawa, Hitoshi Miyasaka
Summary: Host-guest electron transfer is a critical factor for functional changes in molecular framework systems. This study achieved reversible magnetic phase transition by adsorbing iodine and demonstrated a significant enhancement in electrical conductivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Pavel N. Zolotarev
Summary: Through extracting a large number of crystal structures of ionic coordination polymers, the study used machine learning models to predict the relationship between changes in framework topology and changes in extra framework ion properties. The analysis of feature importance in classifiers revealed a set of important ion properties that can affect the changes in corresponding framework characteristics.
CRYSTAL GROWTH & DESIGN
(2021)
Article
Chemistry, Multidisciplinary
Aaron J. Scott, Julia Vallejo, Arup Sarkar, Lucy Smythe, E. Regincos Marti, Gary S. Nichol, Wim T. Klooster, Simon J. Coles, Mark Murrie, Gopalan Rajaraman, Stergios Piligkos, Paul J. Lusby, Euan K. Brechin
Summary: The reaction of Ni(OTf)(2) with the bisbidentate quaterpyridine ligand L leads to the self-assembly of a tetrahedral, paramagnetic cage [(Ni4L6)-L-II](8+). By selectively exchanging the triflate, a series of host-guest complexes with encapsulated paramagnetic tetrahalometallate ions have been prepared. Magnetic susceptibility and magnetisation data suggest comparable and antiferromagnetic magnetic exchange interactions between metal ions in the host complex and the guest species.
Article
Chemistry, Inorganic & Nuclear
Meiling Li, Guojian Ren, Weiting Yang, Yu Fang, Xuanming Zhang, Yu Ma, Shuyan Song, Qinhe Pan
Summary: Researchers have developed a Cd-based MOF as a host to encapsulate both lanthanide ions and carbon quantum dots to achieve multiple fluorescence emissions through modulation of host-guest and guest-guest interactions, showing promise for various anticounterfeiting applications.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Meiling Li, Guojian Ren, Weiting Yang, Yu Fang, Xuanming Zhang, Yu Ma, Shuyan Song, Qinhe Pan
Summary: Developing fluorescent materials with multiple and tunable emissions in MOFs can achieve different modes of fluorescence emission for multiple anticounterfeiting purposes. This research provides a new approach for constructing hybrid MOF-based materials with controlled fluorescence properties for emerging anticounterfeiting applications in various fields.
INORGANIC CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Xue Han, Sihai Yang
Summary: Since its first industrial production in the 1890s, acetylene has been crucial in manufacturing various materials. With the development of functional porous materials, such as metal-organic frameworks and decorated zeolites, there is a growing interest in developing new technologies to improve the safety, energy efficiency, and carbon footprint of acetylene processes. This Minireview explores the applications of these advanced porous materials in acetylene purification and storage, discusses the challenges in developing solid sorbent-based separation technologies, and identifies areas for future research efforts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xue Han, Sihai Yang, Martin Schroder
Summary: Efficient production of ammonia from dinitrogen and water using renewable energy is crucial for the ammonia economy. Functional metal-organic framework (MOF) catalysts have unique properties and show promise in the reduction of N-2 to NH3. By understanding their structure and spectroscopic properties, new advanced catalysts can be developed to produce green NH3. The potential application of MOFs in the capture, storage, and transport of NH3 is also discussed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Physics, Multidisciplinary
M. Krzystyniak, M. J. Gutmann, K. Refson, G. Romanelli, S. Rudic, S. C. Capelli, D. Fortes, O. Magdysyuk, J. I. Marquez Damian, G. Maciel-Pereira
Summary: This study investigates the interplay between phonon anharmonicity and nuclear quantum effects in hexamethylenetetramine (HMT) and its deuterated counterpart (DHMT) using a combination of experimental techniques and theoretical calculations. The results show that the combined effects of isotopic substitution, temperature, anharmonicity, and nuclear quantum effects lead to systematic discrepancies between theoretical predictions and experimental data. Additionally, a significant effect known as the reverse Ubbelohde effect, where deuteration decreases hydrogen bond length in HMT, is observed.
Article
Chemistry, Multidisciplinary
Shouqi Shao, Gareth R. M. Tainton, W. J. Kuang, Nick Clark, Roman Gorbachev, Alexander Eggeman, Irina V. Grigorieva, Daniel J. Kelly, Sarah J. Haigh
Summary: Through the use of 4D scanning transmission electron microscopy (4DSTEM) and energy dispersive X-ray spectroscopy (EDS), it was found that there is structural and chemical heterogeneity, as well as the formation of previously unknown intermediate superstructures, during potassium intercalation and deintercalation processes. The developed in situ correlative STEM-EDS methodology has the potential to determine optimal synthesis, processing, and working conditions for various intercalated or pillared materials.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zi Wang, Alena M. Sheveleva, Daniel Lee, Yinlin Chen, Dinu Iuga, W. Trent Franks, Yujie Ma, Jiangnan Li, Lei Li, Yongqiang Cheng, Luke L. Daemen, Sarah J. Days, Anibal J. Ramirez-Cuesta, Bing Han, Alexander S. Eggeman, Eric J. L. McInnes, Floriana Tuna, Sihai Yang, Martin Schroder
Summary: We have investigated the reactivity modulation of nitrogen dioxide (NO2) by a charged metal-organic framework (MOF) material, MFM-305-CH3. Methylated unbound N-centres and Cl- ions in the pores are used to balance the cationic charge. The uptake of NO2 into MFM-305-CH3 leads to the reaction between NO2 and Cl- to form nitrosyl chloride (NOCl) and NO3- anions. The study provides insights into the binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biotechnology & Applied Microbiology
Jinxin Xie, Victoria S. Coker, Brian O'Driscoll, Rongsheng Cai, Sarah J. Haigh, Jonathan R. Lloyd
Summary: This study found that Geobacter sulfurreducens cannot directly reduce pentavalent antimony or cause its release. The results highlight the close associations between iron and antimony in environmental systems, suggesting the potential use of iron for remediation of antimony contamination.
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Mariana M. Coimbra, Ines Martins, Sofia M. Bruno, Pedro D. Vaz, Paulo J. A. Ribeiro-Claro, Svemir Rudic, Mariela M. Nolasco
Summary: The unique properties of Egyptian blue, a cuprorivaite pigment, were studied using computational and experimental methods. A reliable model of the crystal was obtained, allowing for the evaluation of its lattice dynamics and properties. Inelastic neutron scattering and infrared spectroscopies provided information on the chemical surfaces of the pigment, confirming the simulation results.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Yu Han, Yinlin Chen, Yujie Ma, Jamie Bailey, Zi Wang, Daniel Lee, Alena M. Sheveleva, Floriana Tuna, Eric J. L. McInnes, Mark D. Frogley, Sarah J. Day, Stephen P. Thompson, Ben F. Spencer, Marek Nikiel, Pascal Manuel, Danielle Crawshaw, Martin Schroder, Sihai Yang
Summary: This paper reports the high adsorption of benzene at low pressure and efficient separation of benzene/cyclohexane achieved by controlling the pore chemistry of two families of robust metal-organic frameworks, UiO-66 and MFM-300. UiO-66-CuII exhibits exceptional adsorption of benzene at 3.92 mmol g-1 and MFM-300(Sc) shows a high selectivity of 166 for the separation of benzene/cyclohexane (v/v = 1/1) mixture. The binding mechanisms of benzene and cyclohexane in these materials are revealed through in situ synchrotron X-ray diffraction, neutron powder diffraction, and multiple spectroscopic techniques. Reversible binding of benzene at an open Cu(II) site within metal-organic frameworks is also visualized for the first time.
Article
Chemistry, Multidisciplinary
Lixia Guo, Joseph Hurd, Meng He, Wanpeng Lu, Jiangnan Li, Danielle Crawshaw, Mengtian Fan, Sergei Sapchenko, Yinlin Chen, Xiangdi Zeng, Meredydd Kippax-Jones, Wenyuan Huang, Zhaodong Zhu, Pascal Manuel, Mark D. Frogley, Daniel Lee, Martin Schroeder, Sihai Yang
Summary: The development of stable sorbent materials for reversible adsorption of ammonia is challenging. In this study, the efficient capture and storage of ammonia in four robust aluminium-based metal-organic frameworks were investigated. The results showed that MIL-160 exhibited high ammonia uptake capacity, and the pore geometry, framework rigidity, and host-guest binding sites played a crucial role in determining the ammonia capture and storage capacity.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Computer Science, Artificial Intelligence
Yongqiang Cheng, Geoffrey Wu, Daniel M. Pajerowski, Matthew B. Stone, Andrei T. Savici, Mingda Li, Anibal J. Ramirez-Cuesta
Summary: In this work, a predictive framework based on machine learning is developed to directly predict one-dimensional and two-dimensional inelastic neutron scattering spectra. By using only atomic coordinates as input, high-quality spectra prediction is achieved. This work offers improved efficiency in using limited neutron scattering measurement resources and provides insights into building structure-property relationships in experimental data analysis.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Wenyuan Huang, Qingqing Mei, Shaojun Xu, Bing An, Meng He, Jiangnan Li, Yinlin Chen, Xue Han, Tian Luo, Lixia Guo, Joseph Hurd, Daniel Lee, Evan Tillotson, Sarah Haigh, Alex Walton, Sarah Day, Louise Natrajan, Martin Schroeder, Sihai Yang
Summary: This study reports the direct synthesis of N-formamides by coupling reductive amination of carbonyl compounds and CO2 fixation. A ruthenium catalyst supported by a metal-organic framework was used to achieve highly selective production of N-formamides. The presence of host-guest binding interactions between the catalyst and adsorbed substrates facilitated the activation of substrates and promoted selectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Xi Chen, Sergei Sapchenko, Wanpeng Lu, Ming Li, Meng He, Yinlin Chen, Mark D. Frogley, Ivan da Silva, Sihai Yang, Martin Schroder
Summary: Metal-organic framework (MOF) materials have gained increasing interest in electronics due to their diverse structures, intrinsic porosity, and designable host-guest interactions. In this study, we investigated the dielectric properties of a series of robust materials, MFM-300(M) (M = Al, Sc, Cr, Fe, Ga, In), upon exposure to different guest molecules. We found that MFM-300(Fe) showed the highest increase in dielectric constant when adsorbing NH3, indicating its potential as a powerful dielectric-based sensor for NH3. Structural analysis and spectroscopy confirmed the electron delocalization induced by host-guest interactions between NH3 and the MOF host, resulting in structural polarization and a high dielectric constant.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yujie Ma, Xue Han, Shaojun Xu, Zhe Li, Wanpeng Lu, Bing An, Daniel Lee, Sarayute Chansai, Alena M. Sheveleva, Zi Wang, Yinlin Chen, Jiangnan Li, Weiyao Li, Rongsheng Cai, Ivan da Silva, Yongqiang Cheng, Luke L. Daemen, Floriana Tuna, Eric J. L. McInnes, Lewis Hughes, Pascal Manuel, Anibal J. Ramirez-Cuesta, Sarah J. Haigh, Christopher Hardacre, Martin Schroder, Sihai Yang
Summary: This study presents a method to directly convert methane to ethylene and acetylene using non-thermal plasma under ambient conditions. A cascade fixed-bed system is developed for online separation of the products. The method achieves high selectivity and time yield, providing a new avenue for natural gas utilization.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jin Chen, Bing An, Yinlin Chen, Xue Han, Qingqing Mei, Meng He, Yongqiang Cheng, Inigo J. Vitorica-Yrezabal, Louise S. Natrajan, Daniel Lee, Anibal J. Ramirez-Cuesta, Sihai Yang, Martin Schroder
Summary: Researchers have reported a new metal-organic framework material, MFM-808-SO4, which exhibits high proton conductivity at high humidity and temperature. The material also possesses excellent photocatalytic activity for water splitting to produce hydrogen.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Tian Luo, Zi Wang, Yinlin Chen, Hengzhao Li, Mengqi Peng, Floriana Tuna, Eric J. L. Mcinnes, Sarah J. Day, Jie An, Martin Schroeder, Sihai Yang
Summary: This study reports a method for photocatalytic dehalogenative deuteration using a metal-organic framework, MFM-300(Cr), as the catalyst. The catalyst shows high deuterium incorporation and excellent tolerance to various functional groups. Synchrotron X-ray powder diffraction and in situ electron paramagnetic resonance spectroscopy reveal the mechanism and reaction pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
