Article
Chemistry, Multidisciplinary
Philip M. Stanley, Florian Sixt, Julien Warnan
Summary: This study demonstrates the specific confinement of a rhenium coordination complex in a metal-organic framework (MOF) that enables unique electron accumulating property under visible-light irradiation. The material can concentrate and store electric charges for over four weeks without loss. It also allows decoupled, on-demand discharge for electrochemical reactions and H-2 evolution catalysis. Experimental investigations and theoretical calculations reveal the key role of MOF confinement on molecular guests in electron trapping.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shan-Shan Fu, Qiang-Qiang Yuan, Lihua Ma, Zhi-Ming Zhang, Tong-Bu Lu, Song Guo
Summary: A series of TEMPO@PCN-222 composite photocatalysts were developed by coordinating different amount of 4-carboxy-TEMPO with the secondary building units of PCN-222. Visible-light irradiation enables the transfer of photogenerated holes in the highest occupied molecular orbital of PCN-222 to TEMPO, significantly increasing the photosynthesis of bioactive (iso)quinolones. With an outstanding catalytic stability and substrate tolerance, TEMPO@PCN-222 exhibits a yield of 86.7% for 1-methyl-2-quinolinone, over four times higher than PCN-222 (21.4%). This study provides a new route for constructing composite photocatalysts from abundant starting materials for efficient photosynthesis of high value-added chemicals.
Review
Chemistry, Physical
Juan-Ding Xiao, Rui Li, Hai-Long Jiang
Summary: Metal-organic frameworks (MOFs) are crystalline inorganic-organic hybrid materials with tunable semiconducting behavior. They have potential for use in photocatalysis to produce sustainable solar fuels, thanks to their unique structural advantages that allow for a better understanding of the structure-activity relationship. This review focuses on the active sites in MOF-based photocatalysts and discusses their enhanced activity based on the well-defined structure of MOFs, providing deep insights into MOF-based photocatalysis.
Article
Chemistry, Multidisciplinary
Sixiao Liu, Zhenyuan Teng, Hang Liu, Tianyi Wang, Guoxiu Wang, Qiang Xu, Xiuyun Zhang, Min Jiang, Chengyin Wang, Wei Huang, Huan Pang
Summary: This study investigates a new type of graphene-embedded Ce-based UiO-66 photocatalyst (GSCe) with remarkable nitrogen fixation efficiency under solar light, making it a promising environmentally friendly solar fertilizer for crop cultivation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Peiyu Cai, Ming Xu, Sha-Sha Meng, Zaifeng Lin, Tianhao Yan, Hannah F. Drake, Peng Zhang, Jiandong Pang, Zhi-Yuan Gu, Hong-Cai Zhou
Summary: Efficient photocatalysis in metal-organic frameworks (MOF) and MOF nanosheets (NSs) is limited by short-lived charge separation and self-quenching. Energy-transfer process (EnT) is proposed to enhance charge separation and the catalytic performance of a series of MOF NSs. By utilizing NS, the photocatalyst can be well isolated to reduce self-quenching, leading to enhanced catalytic performances.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Physical
Jun Guo, Yue Wan, Yanfei Zhu, Meiting Zhao, Zhiyong Tang
Summary: MNP/MOF composite photocatalysts exhibit excellent performance and great potential applications, especially in photocatalytic hydrogen production, carbon dioxide reduction, organic transformation reactions, and photodegradation of pollutants. The challenges and prospects in the current research are also proposed and discussed for further advancement in this hot research field.
Article
Chemistry, Physical
Xiaolu Zhao, Chunxin Lu, Linsen Yang, Weipeng Chen, Weiwen Xin, Xiang-Yu Kong, Qiang Fu, Liping Wen, Greg Qiao, Lei Jiang
Summary: Bioinspired nanofluidic devices have great potential in various fields, but face challenges in low energy conversion efficiency and practical application limitations. By designing a heterogeneous membrane structure and incorporating metal organic framework into polymer matrix, high power density and energy conversion efficiency can be achieved.
Article
Energy & Fuels
Chen Li, Zhuo Zhang, Tianyuan Zhong, Guang Wang
Summary: A novel photochromic azo-grafted metal-organic framework (MOF), ZIF-90-AAT, was synthesized and characterized. ZIF-90-AAT not only retains the three-dimensional porous structure of ZIF-90 and high thermal stability, but also has sufficient free space for the isomerization reaction of azobenzene and photo-energy storage ability. ZIF-90-AAT displayed excellent reversible photochromic performance and can release photo-energy absorbed during the isomerization process. This work demonstrated that MOFs can be used in energy storage and expanded the application range of MOF materials.
JOURNAL OF ENERGY STORAGE
(2022)
Review
Chemistry, Inorganic & Nuclear
Meijie Liu, Zipeng Xing, Zhenzi Li, Wei Zhou
Summary: The core-shell metal organic frameworks (MOFs) have shown significant advantages in photocatalytic applications, such as large specific surface areas and low photogenerated electron-hole recombination, which can enhance the photocatalytic efficiency. Common synthesis strategies for core-shell MOF-based materials include one-pot synthesis, in-situ synthesis, self-template method, and layer-by-layer assembly method.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Physical
Yang Liu, Chensi Tang, Min Cheng, Ming Chen, Sha Chen, Lei Lei, Yashi Chen, Huan Yi, Yukui Fu, Ling Li
Summary: POM@MOF composites have been attracting attention in photocatalysis due to their enhanced performance, which benefits from the high specific surface area and long-range ordered structure of MOFs that ensure a uniform distribution of POMs and provide more active catalytic sites.
Article
Chemistry, Physical
Philip M. Stanley, Christopher Thomas, Erling Thyrhaug, Alexander Urstoeger, Michael Schuster, Juergen Hauer, Bernhard Rieger, Julien Warnan, Roland A. Fischer
Summary: This study presents a novel approach to enhance photocatalytic CO2 reduction activity by embedding a molecular catalyst in a metal-organic framework. The ratio of immobilized catalyst to photosensitizer is crucial for improving reaction efficiency and determining optimal performance, while the research also reveals the impact of reaction environment on active sites and provides a future direction for increasing turnover numbers.
Article
Chemistry, Physical
Jaykishon Swain, Anulipsa Priyadarshini, Sugato Hajra, Swati Panda, Jagannath Panda, Raghabendra Samantaray, Yusuke Yamauchi, Minsu Han, Hoe Joon Kim, Rojalin Sahu
Summary: In this study, BaTiO3 nanoparticles are loaded into a Zeolitic Imidazolate Framework (ZIF-8) to create BaTiO3 @ZIF-8 nanocomposites for the photocatalytic degradation of dyes in wastewater. The results demonstrate that the composite efficiently degrades dyes under solar irradiation and exhibits excellent performance.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Environmental Sciences
Xingmao Zhang, Hang Wang, Mingming Gao, Pengfei Zhao, Wenli Xia, Ruile Yang, Yichao Huang, Lin Wang, Mingxu Liu, Tong Wei, Lu Wang, Ruxin Yao, Xiang Li, Zhuangjun Fan
Summary: In this study, a new photocatalyst, pomegranate-shaped zinc oxide@zeolitic imidazolate framework (ZnO@ZIF-8), was successfully prepared for efficient tetracycline degradation under visible light. The photocatalyst exhibited excellent photostability and could be reused multiple times without loss of activity.
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)
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
Eva Loccufier, Geert Watson, Yingrui Zhao, Maria Meledina, Robbe Denis, Parviz Gohari Derakhshandeh, Pascal Van Der Voort, Karen Leus, Damien P. Debecker, Klaartje De Buysser, Karen De Clerck
Summary: The challenge of converting CO2 and H2 into fuels can be addressed by developing a stable, reusable, and easy to handle heterogeneous catalyst. In this study, Ru nanoparticles were encapsulated inside the metal organic framework Cr-MIL-101 and loaded onto a silica nanofibrous membrane. The resulting catalytic membrane showed promising performance for the Sabatier methanation reaction, paving the way for efficient CO2 hydrogenation processes.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Optics
Zetian Yang, Jieqi Hu, David van der Heggen, Mengmeng Jiao, Ang Feng, Henk Vrielinck, Philippe F. F. Smet, Dirk Poelman
Summary: In this study, an all-round dosimeter based on BaMgSiO4, a photochromic material, is reported. The dosimeter exhibits a reversible white-pink color change upon irradiation, making it suitable for dosimetry of X-rays, ultraviolet, and visible light. BaMgSiO4 shows good stability and excellent cycling robustness, making it an ideal choice for integrating detector in various applications. The research findings enhance the understanding of the photochromic behavior in inorganic materials and can stimulate the exploration of new photochromic dosimeters.
LASER & PHOTONICS REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Sander Borgmans, Sven M. J. Rogge, Juul S. De Vos, Pascal van der Voort, Veronique Van Speybroeck
Summary: Soft porous crystals with stimuli responsiveness are widely studied for various applications. However, the structural flexibility in 3D covalent organic frameworks (COFs) is not well understood. This study investigates the factors affecting the phase transformations of diamondoid COFs, including structural decoration, interpenetration, temperature, and guest adsorption. It provides a comprehensive understanding of the design principles for flexible diamondoid COFs.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
L. J. B. Erasmus, P. F. Smet, R. E. Kroon, D. Poelman, J. J. Terblans, J. J. Joos, D. Van der Heggen, H. C. Swart
Summary: Different strontium borate compounds codoped with divalent europium and samarium ions were synthesized using the conventional solid-state reaction method. Optimization of the material was achieved by varying the experimental procedure and the molar ratios of boron and codopants. The optimized material, strontium hexaborate doped with a relatively high europium concentration and a low samarium concentration, exhibited broad excitation range and strong and narrow emission, making it suitable for solar energy generation applications.
Article
Chemistry, Multidisciplinary
Hooman Pazhand, Ali Asghar Sabbagh Alvani, Hassan Sameie, Reza Salimi, Dirk Poelman
Summary: In this research, the controllable synthesis of Metal-organic frameworks (MOFs) with well-defined morphology, composition, and size was studied for understanding their structure-property relationship in various applications. The effect of photocatalyst morphology on optical behavior and photocatalytic efficiency was investigated using physical synthetic parameters for methylene blue removal. The empirical data showed that the particles synthesized at 120 degrees C using iron chloride exhibited the highest efficiency, which can be considered for future research in wastewater treatment.
Article
Chemistry, Multidisciplinary
Amrita Chatterjee, Jiamin Sun, Kuber Singh Rawat, Veronique Van Speybroeck, Pascal van der Voort
Summary: Two donor-acceptor type tetrathiafulvalene (TTF)-based covalent organic frameworks (COFs) were studied as electrodes for symmetric supercapacitors in different electrolytes. The charge storage mechanism of IL electrolyte based supercapacitors depends on the micro pore size and surface charge density of COFs, which can be altered by different electron acceptor building blocks. The combination of these factors enhances the charge storage in highly microporous COFs. DFT calculations support this finding.
Article
Multidisciplinary Sciences
Emile Jules Beckwee, Geert Watson, Maarten Houlleberghs, Daniel Arenas Esteban, Sara Bals, Pascal Van Der Voort, Eric Breynaert, Johan Martens, Gino Baron, Joeri F. M. Denayer
Summary: This study reports a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions and at high water loading. The HR-PMO nanotubes exhibit a steep single-stepped isotherm and a noticeably high methane storage capacity. Supported by ex situ cryo-electron tomography and x-ray diffraction, the findings suggest that HR-PMO nanotubes promote clathrate hydrate nucleation and growth by distributing and confining water in the mesopores of their outer wall, central channels, and external surface. These results highlight the potential application of organosilica materials for pressure-based storage of biomethane in confined clathrate hydrates.
Article
Chemistry, Inorganic & Nuclear
Wanlu Liu, Chunhui Liu, Luca Pilia, Hongliang Zhang, Pascal van der Voort, Anna M. Kaczmarek, Rik Van Deun
Summary: We synthesized a co-condensed hollow ethane-bipyridine periodic mesoporous organosilica (HEt-bpy-PMO) as a host material to anchor lanthanides for developing a multifunctional chemical sensor. The luminescence properties of the developed hybrid materials were studied in detail in the solid-state and after dispersing in water. The Eu3+ or Tb3+ incorporated materials showed ions selectivity towards Cu2+, Co2+, and Fe3+ as ion sensors, and exhibited excellent acetone sensing selectivity.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Jonas Everaert, Karen Leus, Hannes Rijckaert, Maarten Debruyne, Kristof Van Hecke, Rino Morent, Nathalie De Geyter, Veronique Van Speybroeck, Pascal Van Der Voort, Christian V. Stevens
Summary: Covalent triazine frameworks (CTFs) based on polydentate ligands are promising catalyst supports that combine the reactivity of homogeneous catalysts with the robustness and recyclability of heterogeneous ones. In this study, a rhodium (III) complex was immobilized on a bipyridine-based CTF for the transfer hydrogenation of N-heteroarenes in water using sodium formate as the hydrogen source. The immobilized catalyst showed excellent activity for various quinoxalines and other N-heteroarenes, and maintained high activity during recycling, making it suitable for continuous flow synthesis.
Article
Materials Science, Multidisciplinary
Chunhui Liu, Anna M. Kaczmarek, Himanshu Sekhar Jena, Zetian Yang, Dirk Poelman, Pascal van der Voort
Summary: Recent research in lanthanide materials has contributed to the development of chemical sensors, but the current sensors still have limited detection range. We developed lanthanide-based hollow spheres for luminescence turn-off sensing of Hg2+ with low detection limit and wide detection range. This hybrid material exhibited both downshifting and upconversion luminescence.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Maojun Deng, Jiamin Sun, Andreas Laemont, Chunhui Liu, Linyang Wang, Laurens Bourda, Jeet Chakraborty, Kristof Van Hecke, Rino Morent, Nathalie De Geyter, Karen Leus, Hui Chen, Pascal van der Voort
Summary: The photocatalytic activity of crystalline porous covalent organic frameworks (COFs) was significantly enhanced by extending their π-conjugation system through a post-sulfurization process. Thiazole-linked COFs exhibited the best photocatalytic performance, with a rate 5.8 and 3.7 times higher than imine-linked COFs 4PE-N and 4PE-TT, respectively.
Article
Chemistry, Physical
Juul S. De Vos, Sander Borgmans, Pascal Van Der Voort, Sven M. J. Rogge, Veronique Van Speybroeck
Summary: This article introduces a database called ReDD-COFFEE, which contains 268,687 covalent organic frameworks (COFs) with accompanying ab initio derived force fields that outperform generic ones. The database provides a large number of computer-ready structures with high diversity in terms of geometric properties, linker cores, and linkage types. Additionally, the textural properties of the database are analyzed and the most promising COFs for vehicular methane storage are identified. By making the database freely accessible, it is hoped that it can inspire others to further explore the potential of these intriguing functional materials.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Amrita Chatterjee, Linyang Wang, Pascal Van Der Voort
Summary: There is an urgent need for cleaner production processes in the chemical field. Heterogeneous photocatalysis, which converts (visible) light into chemical energy, shows promise as an efficient alternative. Metal-organic frameworks (MOFs) have emerged as a favorable material for photocatalysis due to their large surface area, tunable properties, versatile functionality, and ability to form composites. Research is focusing on constructing Z-scheme heterojunctions in MOFs to enhance light harvesting capacity and improve the redox ability of photocatalysts.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Geert Watson, Nithin B. Kummamuru, Sammy W. Verbruggen, Patrice Perreault, Maarten Houlleberghs, Johan Martens, Eric Breynaert, Pascal van der Voort
Summary: This study explores the use of hydrophobic periodic organosilica nanoparticles for hydrogen storage as clathrate hydrates. The surface decoration with promoter agents enhances the formation and growth kinetics of clathrate hydrates, resulting in an increase in hydrogen storage capacity. These findings are of significant importance for the development of hydrogen clathrates in industrial applications.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
