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, Physical
Marvin Treger, Adrian Hannebauer, Andreas Schaate, Jan L. Budde, Peter Behrens, Andreas M. Schneider
Summary: Metal-organic frameworks (MOFs) with modular design are explored for optical applications, focusing on Zr-based UiO-66 and its derivatives. Novel UiO-66-type MOFs with bifunctional 1,4-benzenedicarboxylate (bdc) linkers are introduced and successfully synthesized. Density functional theory (DFT) and HSE06 hybrid functional calculations are used to study electronic structures and optical properties. The refractive index dispersion of seven UiO-66-type materials is compared, showing the potential for tailored optical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Correction
Chemistry, Physical
Marvin Treger, Adrian Hannebauer, Andreas Schneider, Jan L. Budde, Peter Behrens, Andreas M. Schneider
Summary: The optical properties of the metal-organic framework UiO-66 were tuned by ligand functionalization in this study. The research provides new insights into the optical applications of metal-organic frameworks.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Olesya O. Semivrazhskaya, Daniil Salionov, Adam H. Clark, Nicola P. M. Casati, Maarten Nachtegaal, Marco Ranocchiari, Sasa Bjelic, Rene Verel, Jeroen A. van Bokhoven, Vitaly L. Sushkevich
Summary: By using various experimental techniques, it is shown that the nucleation of UiO-66 occurs through the solution-mediated hydrolysis of zirconium chloroterephthalates, which is autocatalytic. The nuclei of UiO-66 possess the same local environment as the crystals, but lack long-range order, which is gained during the crystallization. Crystal growth is the rate-determining step, while fast nucleation controls the formation of small crystals of UiO-66 with a narrow size distribution of about 200 nanometers.
Article
Chemistry, Multidisciplinary
Victor Charles, Yong Yang, Menglei Yuan, Jitao Zhang, Yaling Li, Jingxian Zhang, Tongkun Zhao, Zhanjun Liu, Bin Li, Guangjin Zhang
Summary: The study demonstrates that CoOx/UiO-66-300 and NiO/UiO-66-300 heterostructures prepared using ultrasonic impregnation show excellent oxygen evolution reaction activities with rapid electron transfer. The calcination temperature significantly affects the stability of the UiO-66 framework and reaction activity.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Engineering, Environmental
Mohua Li, Yanbiao Liu, Fang Li, Chensi Shen, Yusuf Valentino Kaneti, Yusuke Yamauchi, Brian Yuliarto, Bo Chen, Chong-Chen Wang
Summary: The study introduced defects into hierarchical porous metal-organic frameworks (HP-MOFs) to improve their phosphate adsorption performance, using a template-assisted strategy to control the defects. Experimental results demonstrated the critical role of defect sites in enhancing phosphate uptake performance, providing a promising route for tailoring the adsorption performance of MOF-based adsorbents through defect engineering.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Environmental Sciences
Yu-Jen Lee, Ying-Ju Chang, Jyh-Ping Hsu
Summary: UiO-66 metal-organic framework is stable and tolerant to extreme conditions, with the ability to be converted into amorphous derivatives for efficient adsorption capabilities. Doped nucleophiles enhance the adsorption towards Cu(II) and phosphate species through electrostatic interactions and hydrogen bonding.
Article
Engineering, Environmental
Azam Jalali, Ali Ahmadpour, Mahboube Ghahramaninezhad, Elham Yasari
Summary: A new nanocomposite with enhanced CO2 adsorption capacity, thermal stability, and selectivity has been synthesized and studied. The nanocomposite showed a significant improvement in CO2 adsorption capacity compared to pristine UiO-66. It also exhibited good thermal stability and reversibility. This nanocomposite has potential applications in biogas and natural gas purification.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Applied
Alexandre M. Viana, Diana Juliao, Fatima Mirante, Rui G. Faria, Baltazar de Castro, Salete S. Balula, Luis Cunha-Silva
Summary: A novel chloride activation method was developed to enhance the catalytic activity of UiO-66(Zr) and UiO-66(Hf) materials in oxidative desulfurization reactions. The activation treatment significantly improved the catalytic performance of the materials, even after multiple reaction cycles, without structural degradation of the catalyst. This cost-effective method shows promise for efficiently activating catalytic MOF materials and expanding their catalytic applications.
Article
Nanoscience & Nanotechnology
Alexandra Loosen, Charlotte Simms, Simon Smolders, Dirk E. De Vos, Tatjana N. Parac-Vogt
Summary: Tuning the Ce/Zr metal ratio in MOFs is a promising strategy to improve catalytic activity, increase efficiency in peptide hydrolysis and oxidation, broaden reaction scope, and enhance adsorption of dipeptides. The introduction of Ce enhances the reactivity of MOFs and their potential in various biologically relevant reactions.
ACS APPLIED NANO MATERIALS
(2021)
Article
Chemistry, Inorganic & Nuclear
Guodong Fu, Ping Wu, Shiping Zhang, Li Wang, Min Xu, Xiulan Huai
Summary: Post-synthetic modification is an effective method for structural replacement or functional modification of materials. In this study, organic ligands with N-functionalities or amino groups were introduced into defective UiO-66 through post-synthetic ligand exchange (PSE) to improve its water adsorption performance.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Zhixiong Guo, Qian-Cheng Luo, Lei Qin, Zhimin Tian, Yan-Zhen Zheng, Yuanyuan Ma, Yongquan Qu
Summary: External stimuli-responsive phase transition of metal-organic frameworks (MOFs) introduces intriguing functions for diverse applications. In this study, a phase transition from cubic Ce-UiO-66 to triclinic Ce-BDC-OH under light irradiation was reported, and the phase transition mechanism involving photoreduction and hydroxylation processes was revealed. The study also highlighted the potential application of the phase transition as a photostimulus-responsive magnetic switch.
INORGANIC CHEMISTRY
(2022)
Article
Environmental Sciences
Huahui Yuan, Juncheng Li, Lejie Pan, Xin Li, Yue Yuan, Qinmei Zhong, Xian Wu, Jin Luo, Sheng-Tao Yang
Summary: This study investigates the particulate toxicity of UiO-66, a representative MOF material, on a model microorganism. The results show that UiO-66 nanoparticles have low toxicity and only cause mild mechanical damage to the fungi.
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
(2022)
Article
Engineering, Chemical
Zhimin Guo, Nan Li, Shixiang Zuo, Chenghong Qiang, Wei Zhan, Zhengping Li, Jiangquan Ma
Summary: Piezoelectric materials, such as UiO-66, have shown promising potential in catalyzing the sustained removal of pollutants. In this study, the introduction of the polar molecule adenine in the synthesis process of UiO-66 led to enhanced piezoelectric properties and structure asymmetry. The optimized catalyst, AD U, exhibited improved piezoelectric potential and charge separation efficiency compared to UiO-66. Additionally, AD U demonstrated enhanced piezoelectric degradation efficiency for diclofenac sodium (DCF) compared to pure UiO-66, and the major role of h+ in destroying DCF molecules was confirmed through experiments. Three possible degradation pathways for DCF were proposed using DFT and LC-MS. This work provides a new pathway to enhance the piezoelectric properties of MOFs and expands their applications in the field of piezocatalysis.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Vasily Gvilava, Maximilian Vieten, Robert Oestreich, Dennis Woschko, Moritz Steinert, Ishtvan Boldog, Roman Bulanek, Natalie A. Fokina, Peter R. Schreiner, Christoph Janiak
Summary: The first use of a bulky barrel-shaped ligand in HHUD-3 is demonstrated, which shows accessible porosity only feasible for a defect structure. With 35%+ missing linker defects and S-BET = 890 m(2)g(-1) (N-2), HHUD-3 exhibits higher CH4 adsorption but lower CO2 and H-2 adsorption compared to UiO-66.
Article
Chemistry, Inorganic & Nuclear
Debmalya Ray, Meagan S. Oakley, Arup Sarkar, Xiaojing Bai, Laura Gagliardi
Summary: By computationally exploring the electronic structure and magnetic properties of a hypothetical Cf(III) complex, we found that it can behave as a single molecule magnet (SMM) with higher magnetic susceptibility compared to other early-actinide-based magnetic complexes. However, due to alpha-decay, Cf can convert to Cm and affect its SMM behavior. Additionally, the study suggests that the ligand field is dominant in Cf(III), which significantly increases its magnetization blocking barrier compared to its 4f congener.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tyler M. VanOursouw, Trevor Rottiger, Kiley A. Wadzinski, Brian E. VanderWaal, Madison J. Snyder, Riley T. Bittner, Omar K. Farha, Shannon C. Riha, Joseph E. Mondloch
Summary: A two-component undergraduate laboratory experience was developed by students in a senior level capstone course. The first component involved the rapid synthesis of a metal-organic framework (MOF-808) in aqueous solution. The second component included the characterization of MOF-808 using various instruments, as well as quantifying the adsorption of PFAS from solution. This laboratory experience provides students with the opportunity to synthesize a modern porous solid and explore its potential applications in MOF science.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Chemistry, Multidisciplinary
Sajal Sen, Fumitaka Ishiwari, Ramandeep Kaur, Masatoshi Ishida, Debmalya Ray, Koichi Kikuchi, Takehiko Mori, Steffen Bahring, Vincent M. Lynch, Akinori Saeki, Dirk M. Guldi, Jonathan L. Sessler, Atanu Jana
Summary: We reported the synthesis of a nanosized buckytrap, constructed from two bis-zinc(II) expanded-TTF (exTTF) porphyrin subunits, which could form discrete host-guest inclusion complexes with fullerenes. The axial ligands of the nanosized buckytrap determined the formation of either discrete complexes or infinite organic frameworks. Emission spectroscopic studies and flash-photolysis time-resolved microwave conductivity (FP-TRMC) studies revealed the binding stoichiometry and photoconductivity of the complexes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Yongwei Chen, Karam B. Idrees, Mohammad Rasel Mian, Florencia A. Son, Chenghui Zhang, Xingjie Wang, Omar K. Farha
Summary: In this study, a Zr-based MOF, NU-600, was used to demonstrate the construction of multi-component MOFs with unprecedented complexity and control by inserting two linear linkers with different lengths into distinct pockets. It was found that increasing the connectivity of Zr6 nodes remarkably reinforced the hydrolytic stability of these linker-inserted MOFs while maintaining their water uptake capacity and pore-filling pressure. Additionally, introducing hydrophilic -OH groups into the linkers effectively shifted the pore-filling step to lower partial pressures. This methodology provides a powerful strategy to enhance the structural stability of other MOF frameworks and promotes advancements in fundamental sciences and practical applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chen Wang, Heyao Zhang, Yao Wang, Jie Wu, Kent O. Kirlikovali, Peng Li, Yaming Zhou, Omar K. Farha
Summary: A general and efficient strategy is reported for the synthesis of inverse opal metal-organic frameworks (IO MOFs) with tunable macro-, meso-, and micro-pores. These materials demonstrate improved adsorption and hydrolysis performance for organophosphorus aggregates.
Article
Chemistry, Physical
Saumil Chheda, WooSeok Jeong, Nikita Hanikel, Laura Gagliardi, J. Ilja Siepmann
Summary: Atmospheric water harvesting using nanoporous sorbent materials has emerged as a potential solution for global water crisis. This study investigates the adsorption behavior of two high-performing metal-organic frameworks (MOFs), MOF-303 and MOF-333, through simulation. The results show that simulations with nonpolarizable force fields and rigid framework structures optimized using electronic structure calculations can achieve good agreement with experimental data, but for MOF-303, a structure accounting for the distortion associated with adsorbed water is necessary.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Shengyi Su, Xuhao Zhou, Xinyi Gong, Karam B. Idrees, Kent O. Kirlikovali, Timur Islamoglu, Omar K. Farha, Nathan C. Gianneschi
Summary: In this study, micro-porous synthetic allomelanin (AM) was used as a porous coating on the surface of the MOF material UiO-66. The core-shell structured AM@UiO-66 nanoparticles were successfully prepared through in situ surface-constrained oxidative polymerization. Nitrogen sorption isotherms confirmed that the AM coating did not affect the pore size and porosity of UiO-66. It was demonstrated that by tuning the thickness of the AM coating, the AM@UiO-66 composites exhibited excellent hexane isomer separation selectivity and storage capacity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Chung -Wei Kung, Ken-ichi Otake, Riki J. Drout, Subhadip Goswami, Omar K. Farha, Joseph T. Hupp
Summary: Starting with ferrocyanide ions in acidic aqueous solution, cyano-ferrate(II) species are post-synthetically grafted to the nodes of a mesoporous zirconium-based MOF, NU-1000. The grafting occurs by substitution of cyanide ligands by node-based hydroxo and oxo ligands rather than by substitution of node aqua ligands by cyanide ligands as bridges between Fe(II) and Zr(IV). The installed moieties yield a broad absorption band that is tentatively ascribed to iron-to-zirconium charge transfer. Consistent with Fe(III/II) redox activity, a modest fraction of the installed iron complexes are directly electrochemically addressable.
Article
Materials Science, Multidisciplinary
Enes Ibrahim Duden, Kubra Gurcan Bayrak, Mert Balkan, Niyaz Cakan, Arsen Demiroglu, Erhan Ayas, Mujdat Caglar, Servet Turan, Timur Islamoglu, Omar K. Farha, Mustafa Erkartal, Unal Sen
Summary: Metal-organic framework (MOF)-derived nanocarbons have been used as reinforcement phase in ceramic composites for the first time. The composite exhibits increased fracture toughness and room-temperature electrical conductivity compared to alumina monoliths. This study demonstrates the potential of MOF-derived nanocarbons for enhancing the mechanical and electrical properties of ceramic matrix composites.
ACS MATERIALS LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Julia G. Knapp, Maksim Y. Livshits, J. Connor Gilhula, Sylvia L. Hanna, Ida D. Piedmonte, Natalie T. Rice, Xingjie Wang, Benjamin W. Stein, Stosh A. Kozimor, Omar K. Farha
Summary: This study investigated the impact of linker identity and photoexcitation on the photocatalytic performance of uranyl-based MOFs. By analyzing the structural and photochemical properties of three uranyl-based MOFs, the study showed that the photophysical properties of linkers can be used to predict the photocatalytic behavior of uranyl-containing MOFs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Chemistry, Multidisciplinary
Zhijie Chen, Kent O. Kirlikovali, Le Shi, Omar K. Farha
Summary: Functional porous metal-organic frameworks (MOFs) have great potential applications in various fields, but their successful implementation depends on their stability. In this article, we summarize the progress in rational design and synthesis of stable and controllable porous MOFs. The reticular synthesis approach allows for the top-down design of stable MOFs with targeted networks and pores. We highlight the synthesis and applications of stable MOFs based on high valent metal ions with carboxylate ligands and low valent metal ions with azolate linkers.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Multidisciplinary
Sylvia L. Hanna, Omar K. Farha
Summary: Uranium, a relatively unexplored element, has rich chemistry and shows promise for various powerful functions such as small molecule activation and photocatalysis. By using metal-organic frameworks (MOFs), researchers have harnessed the properties of uranium and discovered remarkable structures and unique properties not observed in traditional transition metal MOFs. Theoretical calculations have also complemented structure-property studies in uranium MOFs. In this Perspective, the energy-structure-property relationships in U-MOFs are summarized to enable a deeper understanding of chemical phenomena and elevate the field to targeted discovery.
Article
Chemistry, Multidisciplinary
Kaikai Ma, Yuk Ha Cheung, Kent O. Kirlikovali, Xiaoliang Wang, Timur Islamoglu, John H. Xin, Omar K. Farha
Summary: The importance of developing functional materials to protect against chemical and pathogen threats is highlighted by the SARS-CoV-2 pandemic and the misuse of toxic chemical warfare agents. Metal-organic frameworks (MOFs) have emerged as a class of heterogeneous catalysts capable of rapidly detoxifying harmful chemicals and biological hazards. This Account describes the evolution of MOF/fiber composites that effectively capture and deactivate these toxic species, and focuses on key design challenges and considerations.
ACCOUNTS OF MATERIALS RESEARCH
(2023)
Article
Polymer Science
Emily R. Mcclure, Pradipta Das, Karam B. Idrees, Dahee Jung, Omar K. Farha, Julia A. Kalow
Summary: This study demonstrates a method for synthesizing unique ladder polymers with sp3 backbones under mild reaction conditions using photoredox catalysis. By designing specific monomers, the polymerization reaction can take place and high molecular weight products can be obtained. The resulting products can also be utilized to form ladder bottlebrush polymers.
Article
Nanoscience & Nanotechnology
Kent O. Kirlikovali, Sylvia L. Hanna, Florencia A. Son, Omar K. Farha
Summary: This article provides an overview of the design strategies for metal-organic frameworks (MOFs) and discusses how fundamental chemistry concepts are used to synthesize highly crystalline MOFs. It also explores the future possibilities of advanced structures with tailored properties in the MOF field.
ACS NANOSCIENCE AU
(2023)
