Article
Chemistry, Multidisciplinary
Shi-Qiang Wang, Shaza Darwish, Michael J. Zaworotko
Summary: This study reports the variable switching behavior of a previously known square lattice topology coordination network in response to different gaseous adsorbates.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Belen Lerma-Berlanga, Carolina R. Ganivet, Neyvis Almora-Barrios, Sergio Tatay, Yong Peng, Josep Albero, Oscar Fabelo, Javier Gonzalez-Platas, Hermenegildo Garcia, Natalia M. Padial, Carlos Marti-Gastaldo
Summary: Metal-Organic Frameworks are used as crystalline matrices to synthesize multiple component or multivariate solids, allowing for property customization. By optimizing synthesis through high-throughput methods, it is possible to create multivariate frameworks with efficient light sensitization, chemical stability, and porosity for photocatalysis applications. Solvent-assisted linker exchange reactions can control the distribution of linkers in crystals, affecting their performance in photocatalytic activities.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Timur Ashirov, Julya Stein Siena, Mengru Zhang, A. Ozgur Yazaydin, Markus Antonietti, Ali Coskun
Summary: This study demonstrates light-switchable gas separation membranes based on polymeric carbon nitride with fast response times and efficient separation performance.
NATURE COMMUNICATIONS
(2022)
Article
Materials Science, Multidisciplinary
Anastasia Permyakova, Alshaba Kakar, Jonathan Bachir, Effrosyni Gkaniatsou, Bernard Haye, Nicolas Menguy, Farid Nouar, Christian Serre, Nathalie Steunou, Thibaud Coradin, Francisco M. Fernandes, Clemence Sicard
Summary: The mesoporous iron polycarboxylate MIL-100(Fe) was synthesized with the presence of Pseudomonas putida bacteria. The synthesis was done under green conditions, using pure aqueous media at 30 degrees C to ensure the integrity of the cell membrane. The resulting biohybrid showed a unique microstructure, with an exoskeleton encapsulating individual bacteria cell, suggesting strong interactions between the exopolysaccharides network and MOF precursors.
ACS MATERIALS LETTERS
(2023)
Article
Environmental Sciences
Jin Zhong, Xin Yuan, Jun Xiong, Xiaoling Wu, Wenyong Lou
Summary: The accumulation of antibiotics in water poses a great threat to human and ecological health, leading to the development of porous materials for antibiotic removal. Researchers have successfully constructed mesoporous zirconium based metal-organic frameworks (Zr-MOFs) using a simple solvent-dependent strategy. The synthesized MOFs' porous structure was determined by regulating the ratio of water to N, N-dimethylacetamide during synthesis. The obtained Zr-MOF exhibited high adsorption capacity towards tetracycline (TC) and the adsorption mechanism was mainly attributed to the abundant Zr-OH groups and hydrogen bonding interaction between TC and Zr-MOF.
ENVIRONMENTAL RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Jueyi Xue, Mengnan Zhang, Joel Yong, Qianfan Chen, Joseph Wang, Jiangtao Xu, Kang Liang
Summary: This study reports a biocatalytic nanomotor based on a covalent-organic framework (COF) that exhibits intelligent and switchable motion triggered by a blue-to-red light switch. The nanomotor enhances contaminant removal in aqueous solutions when exposed to blue light, but deactivates its motion and contaminant removal under red light. The study explores the assembly strategy of the COF-based nanomotor and its light-controlled propulsion performance, providing insights for the design and practical applications of nanomotors.
Article
Chemistry, Physical
Xinyao Wang, Runping Ye, Melis S. Duyar, Cameron Alexander Hurd Price, Hao Tian, Yanping Chen, Na Ta, Hao Liu, Jian Liu
Summary: In this study, mesoporous ZnCoSiOx hollow nanoreactors with different metal distributions and microenvironment were designed based on the diffusion behavior of metal species in confined nanospace. By using core@shell structured ZnCo-zeolitic imidazolate framework (ZIF)@SiO2 as a template and employing different synthesis methods, double-shelled hollow structures with well-distributed metal species and yolk@shell structures with a collective (Zn-Co) metal oxide as the yolk were successfully obtained. The catalytic performance of these nanoreactors in CO2 hydrogenation showed that the dispersion and location of active sites in the catalysts play a crucial role in determining the main products.
Article
Chemistry, Multidisciplinary
Wei Ru, Yanan Liu, Baoai Fu, Fengzhi Fu, Junting Feng, Dianqing Li
Summary: The study presents a method to activate single Pd atom catalyst through an in situ adsorbate-induced strategy, which involves changing the lattice parameters of MOF materials to control localized electronic states, resulting in a Pd single atom catalyst with high intrinsic activity, selectivity, and long-term stability.
Article
Chemistry, Multidisciplinary
Zehao Zhou, Jian Zhao, Zhenghan Di, Bei Liu, Zhaohui Li, Xuemin Wu, Lele Li
Summary: A mesoporous MOF shell was synthesized on the surface of gold nanorods to capture single AuNRs for combinational phototherapy against solid tumors. The core-shell heterostructures combine a mesoporous structure and photoinduced singlet oxygen generation behavior with plasmonic photothermal conversion characteristic of AuNRs, enabling an efficient tumor treatment strategy. Applications beyond cancer therapy, such as plasmonic harvesting of light energy for catalytic reactions within MOFs and multifunctional nanocarriers for agricultural formulations, are also highlighted.
Article
Chemistry, Physical
Dylan M. Anstine, Dai Tang, David S. Sholl, Coray M. Colina
Summary: This study explores the adsorption space of microporous polymers using molecular simulation data, considering factors such as flexibility to derive correlations for adsorbent swelling and performance. The research identifies high-performing adsorbent systems based on the separation selectivity of distinct binary molecular pairs.
NPJ COMPUTATIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Hua-Qiao Tan, Zhen-Hui Kang, Yang-Guang Li, Tian-Yu Qiu, Ying-Nan Zhao, Wen-Si Tang, Hui-Ying Sun, Xia Zhao
Summary: To conveniently control photocatalytic reactions, the design and development of smart photocatalysts that can be regulated by external stimuli has attracted interest. In this study, a smart imine covalent-organic-framework (COF) photocatalyst was prepared and demonstrated to have switchable photocatalytic properties and efficient sulfide oxidation via proton-initiated reactions.
Article
Multidisciplinary Sciences
Yu Zhang, Long-Zhang Dong, Shan Li, Xin Huang, Jia-Nan Chang, Jian-Hui Wang, Jie Zhou, Shun-Li Li, Ya-Qian Lan
Summary: The study demonstrates that the ECR selectivity depends strongly on the Cu site coordination environment in crystalline porous catalysts, with Cu-DBC showing higher selectivity and activity due to the lower energy barriers of Cu-O-4 sites during the ECR process. This provides a platform for constructing highly selective ECR catalysts with potential applications in the energy conversion field.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Jin Liu, Xingyu Liu, Qi Liu, Jing Cao, Xinheng Lv, Shaoru Wang, Tian Tian, Xiang Zhou, Hexiang Deng
Summary: This study demonstrates the ability of a metal-organic framework (MOF) with mesopores to include and manipulate nucleic acids for bioactivity regulation. The researchers designed and synthesized two MOFs with mesopores and isolated metal sites, which facilitate the entrance of RNA and catalyze the cleavage of carbonate groups. By using the Pd-MOF-626 catalyst, the conversion of RNA is achieved efficiently and the MOF crystals can be easily removed from the reaction media, leaving a minimal metal footprint. These findings suggest the potential of MOF for bioorthogonal chemistry.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Maite Perfecto-Irigaray, Garikoitz Beobide, Sofia Calero, Oscar Castillo, Ivan da Silva, Juan Jose Gutierrez-Sevillano, Antonio Luque, Sonia Perez-Yanez, Leticia F. Velasco
Summary: UiO-66, a metal-organic framework reported in 2008, remains a highly studied MOF due to its exceptional stability. By altering building blocks or employing defect engineering, new topologies can be accessed. The amino functionalization of EHU-30 series enhances its adsorption capabilities for CO2 and water vapor, making it a promising candidate for gas capture and water harvesting applications.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Bo Li, Xiao Liu, Bin Lei, Haiqiang Luo, Xize Liu, Hengzhi Liu, Qinfen Gu, Jian-Gong Ma, Peng Cheng
Summary: Catalytic conversion of CO2 into high value-added chemicals using renewable energy is a challenging task. A new family of 1D dual-channel heterowires, Cu NWs@MOFs, has been developed for electro-/photocatalytic CO2 reductions. By changing the type of MOF cover, the heterowire can switch between electrocatalyst and photocatalyst, achieving excellent selectivity and adjustable products. With high stability, this heterowire offers a promising solution for CO2 reduction.
Article
Chemistry, Physical
Tom Boenke, Sebastian Kirchhoff, Florian S. Reuter, Florian Schmidt, Christine Weller, Susanne Dorfler, Kai Schwedtmann, Paul Hartel, Thomas Abendroth, Holger Althues, Jan J. Weigand, Stefan Kaskel
Summary: Lithium-sulfur (Li-S) batteries have high theoretical specific energy and are promising for lightweight applications like aviation and heavy electric vehicles. However, their rate capability needs improvement. This study evaluates a combination of sparingly polysulfide solvating electrolyte and highly conductive carbon nanotube Buckypaper (CNT-BP) and finds that the sparingly polysulfide solvating electrolyte has better rate capability. This evaluation is an important step towards customizing Li-S batteries for practical applications.
Article
Chemistry, Multidisciplinary
Yiran Liu, Meng Zhao, Li-Peng Hou, Zheng Li, Chen-Xi Bi, Zi-Xian Chen, Qian Cheng, Xue-Qiang Zhang, Bo-Quan Li, Stefan Kaskel, Jia-Qi Huang
Summary: Using dimethyl diselenide (DMDSe) as a redox comediator can enhance the sulfur redox kinetics and suppress the parasitic reactions in Li-S batteries, resulting in high energy density and long cycling stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Irena Senkovska, Volodymyr Bon, Leila Abylgazina, Matthias Mendt, Jan Berger, Gregor Kieslich, Petko Petkov, Jhonatan Luiz Fiorio, Jan-Ole Joswig, Thomas Heine, Larissa Schaper, Christopher Bachetzky, Rochus Schmid, Roland A. A. Fischer, Andreas Poeppl, Eike Brunner, Stefan Kaskel
Summary: Flexible porous frameworks are a cutting-edge area of materials research due to their ability to adaptively open and close pores induced by chemical and physical stimuli, offering a wide range of functions. However, the factors influencing the switchability are still poorly understood, including the role of building blocks, crystal size, defects, cooperativity, and host-guest interactions. This review discusses an integrated approach using idealized model materials to systematically investigate and understand the critical factors affecting framework dynamics, leading to progress in their understanding and application.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Yutong Luo, Leonid Shupletsov, Maria Rita Vega, Adrian Gutierrez-Serpa, Arafat Hossain Khan, Eike Brunner, Irena Senkovska, Stefan Kaskel
Summary: By combining conductive MOFs with CNTs, the electrocatalytic performance for glucose detection can be enhanced, leading to the design of advanced nonenzymatic glucose sensors.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Ahmed G. Attallah, Volodymyr Bon, Kartik Maity, Eric Hirschmann, Maik Butterling, Andreas Wagner, Stefan Kaskel
Summary: Atmospheric water harvesting using metal-organic frameworks (MOFs) is a promising technology for providing clean and long-term water supply in arid areas. In-situ positron annihilation lifetime spectroscopy (PALS) has been utilized to understand the water sorption mechanism in MOFs and select suitable candidates for desired applications. This study investigated the DUT-67-Zr and DUT-67-Hf frameworks using PALS, revealing the stepwise pore filling mechanism of water molecules in MOFs and offering insights for the design and use of MOFs for water harvesting.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Niklas Unglaube, Marc Florent, Thomas Otto, Adrian Gutierrez-Serpa, Markus Stoetzer, Julia Grothe, Stefan Kaskel, Teresa J. Bandosz
Summary: Activated carbon with modified surface chemistry and porosity effectively removes formaldehyde at room temperature. The addition of nitrogen enhances the adsorption capacity, particularly in ultramicropores, increasing the utilization of the carbon surface.
Article
Chemistry, Multidisciplinary
Sattwick Haldar, Arafat H. Khan, Ankita De, Fanny Reichmayr, Ahiud Morag, Minghao Yu, Andreas Schneemann, Stefan Kaskel
Summary: In this study, sulfur is covalently integrated into a polymer through a chemical reaction, enabling it to be used as an electrode material in batteries. This novel electrode material mitigates the dissolution and shuttle effect of sulfur in the batteries, leading to improved cycling stability and reduced overpotential.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Muhammad Fernadi Lukman, Matthias Mendt, Volodymyr Bon, Stefan Kaskel, Andreas Poeppl
Summary: By using paramagnetic Ni2+-Co2+ pairs as spin probes, in situ continuous wave electron paramagnetic resonance investigation has been proven as a powerful method to follow the isotope-selective gate opening phenomenon on the DUT-8(Ni-0.98 Co-0.02) framework. This method is sensitive to the phase transition from closed pore to open pore phase in response to D-2 adsorption, while no phase transformation has been observed during H-2 gas adsorption. Additionally, it can sense local structural changes around the spin probe during D-2 gas desorption. Based on these evidences, the in situ continuous wave electron paramagnetic resonance method can be implemented as an efficient and non-invasive technique for the detection of dihydrogen isotopes.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Alexander E. J. Hoffman, Irena Senkovska, Leila Abylgazina, Volodymyr Bon, Veronika Grzimek, Anna Maria Dominic, Margarita Russina, Marvin A. Kraft, Inez Weidinger, Wolfgang G. Zeier, Veronique Van Speybroeck, Stefan Kaskel
Summary: This study utilizes spectroscopic techniques and density functional theory calculations to investigate the vibrational properties of DUT-8(M) materials with different metal nodes (M = Ni, Co, Zn, Cu). Experimental results show that the closed pore phase of the Ni-based compound is stiffer than those containing Co and Zn, while the open pore phase is softer. Theoretical calculations suggest that changing the metal atom mainly affects the phonon modes inducing changes in the paddle wheel unit. These findings provide valuable insights into the flexibility and phase transition mechanism of switchable MOFs.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Aizhamal Subanbekova, Varvara I. Nikolayenko, Andrey A. Bezrukov, Debobroto Sensharma, Naveen Kumar, Daniel J. O'Hearn, Volodymyr Bon, Shi-Qiang Wang, Kyriaki Koupepidou, Shaza Darwish, Stefan Kaskel, Michael J. Zaworotko
Summary: In this study, a novel 8-fold interpenetrated diamondoid metal-organic framework (MOF) with reversible single-crystal-to-single-crystal transformations and variable pore sizes was synthesized and characterized. The framework exhibited different phases depending on the synthesis and activation conditions, with varying cell volumes and void space. The sorption properties of the MOF were also investigated, showing a water vapor-induced structural transformation and CO2-induced expansion of the unit cell volume. The MOF demonstrated hydrolytic stability and retained its working capacity after multiple cycles of sorbent regeneration.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Bodo Felsner, Volodymyr Bon, Christopher Bachetzky, Eike Brunner, Stefan Kaskel
Summary: Predictive design of guest-responsive frameworks on the molecular level remains a major challenge for chemists. The isoreticular approach is a promising method for designing MOFs with desired properties. In this study, the isoreticular approach was successfully applied to design new flexible frameworks, and their flexibility mechanisms were explored using various methods. The findings can serve as a roadmap for discovering new flexible frameworks with desired properties.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Physical
Michelle Ernst, Jack D. Evans, Ganna Gryn'ova
Summary: The performance of metal-organic and covalent organic framework materials in important applications such as gas capture, storage, and separation heavily relies on the interactions established inside their pores. Computational modeling provides detailed information about these interactions at a level of precision often unachievable through experiments. The review summarizes key simulation techniques, presents examples of their use in organic framework hosts analysis and design, and discusses high-throughput screening and machine learning techniques for predicting their properties and performances.
CHEMICAL PHYSICS REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Josephine F. Smernik, Pol Gimeno-Fonquernie, Jorge Albalad, Tyla S. Jones, Rosemary J. Young, Neil R. Champness, Christian J. Doonan, Jack D. Evans, Christopher J. Sumby
Summary: This study investigates the synthesis of Mn-based metal-organic frameworks (MOFs), finding that MnMOF-1 is a kinetic or metastable phase, while a newly identified 2D layered material, MnMOF-2D, is the thermodynamically favored product. It is also shown that using longer linkers can help to form more stable structures. In addition, two new porous 3D Mn-based MOFs were successfully synthesized, highlighting the viability of using tetratopic hinged linkers to form 3D MOFs.
Article
Electrochemistry
Florian S. Hoffmann, Florian Schmidt, Jannes Mueller, Kay Schoenherr, Susanne Doerfler, Thomas Abendroth, Holger Althues, Arno Kwade, Nae-Lih Wu, Stefan Kaskel
Summary: A new low density electrolyte based on hexyl methyl ether (HME) and 1,3-dioxalane (DOL) is presented in this study, which allows the use of graphite as anode material for Li-S batteries. The electrolyte showed a high Coulombic efficiency in graphite vs. graphite cells. Additionally, the cycling conditions for Li-S cells with graphite anodes were optimized for the first time.
BATTERIES & SUPERCAPS
(2023)
