Article
Chemistry, Multidisciplinary
Johannes Hungwe, Piwai Tshuma, Maureen Gumbo, Francoise M. Amombo Noa, Lars Ohrstrom, Gift Mehlana
Summary: Two new metal-organic frameworks, MSU-10 and MSU-11, based on 2,2'-bipyridine-4,4'-dicarboxylate and La(III) ions, were synthesized under solvothermal conditions. MSU-10 is a 2D network structure, while MSU-11 is a 3D network structure exhibiting an unusual rod-MOF topology zbj, obtained by introducing a modulator, 1,10-phenanthroline. Both networks are stable upon guest removal, but show phase change after soaking in solvents for 24 hours. Network analysis revealed that MSU-11 is isoreticular with MOF-80 constructed with different linkers and metal ions.
Article
Chemistry, Multidisciplinary
Qihao Yang, Yinming Wang, Xuan Tang, Qiuju Zhang, Sheng Dai, Huaitao Peng, Yichao Lin, Ziqi Tian, Zhiyi Lu, Liang Chen
Summary: This article demonstrates the precise regulation of ligand defect density in metal-organic frameworks by tuning linker groups. The ligand defect density is positively correlated with the electronegativity of linker groups. Metal-organic frameworks with high ligand defect density exhibit improved catalytic performance.
Article
Chemistry, Physical
Yushan Chen, Jiakun Wang, Zebin Yu, Yanping Hou, Ronghua Jiang, Mi Wang, Jun Huang, Jianhua Chen, Yongqing Zhang, Hongxiang Zhu
Summary: A novel non-precious metal bifunctional electrocatalyst with lattice strain was developed and showed excellent catalytic performance in overall water splitting. The lattice strain effectively facilitated electron transfer and enhanced the activity of the catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Multidisciplinary Sciences
Ryunosuke Hayashi, Shohei Tashiro, Masahiro Asakura, Shinya Mitsui, Mitsuhiko Shionoya
Summary: The structure of porous molecular crystals can be controlled allosterically by the adsorption of effectors within low-symmetry nanochannels with multiple molecular recognition sites, leading to diverse framework structure conversion and switchable molecular affinity at different recognition sites. These findings may provide guidance for the development of supramolecular materials with flexible and highly-ordered three-dimensional structures for biological applications.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Kenton E. Hicks, Andrew T. Y. Wolek, Omar K. Farha, Justin M. Notestein
Summary: This study investigates the influence of thermal pretreatments and MOF topology on the activity of Zr6O8 cluster in Zr-MOFs. The results show that both factors affect the acidity of protons generated from H2 activation and their resulting activity for olefin conversion. The geometry of open coordination sites on individual Zr6O8 nodes also influences butene hydrogenation. These findings underscore the importance of pretreatment and MOF topology in defining MOF catalytic activity.
Article
Chemistry, Multidisciplinary
Ling Zhang, Jiaji Wang, Ke Jiang, Zhaohui Xiao, Yuntian Gao, Shiwei Lin, Banglin Chen
Summary: A steady self-reconstructed MOF heterojunction with greatly improved OER activity and superior durability has been constructed through redox electrochemistry and topology-guided strategy.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Kenton E. Hicks, Andrew T. Y. Wolek, Omar K. Farha, Justin M. Notestein
Summary: This study investigates the influence of thermal pretreatments and MOF topology on the activity of Zr6O8 clusters for H-2 activation and 1-butene hydrogenation and isomerization. The results show that both thermal pretreatment and MOF topology affect the acidity of protons generated from H-2 activation and their resulting activity for olefin conversion. Additionally, the geometry of open coordination sites on individual Zr6O8 nodes influences butene hydrogenation.
Article
Engineering, Environmental
Siti Zu Nurain Ahmad, Wan Norharyati Wan Salleh, Nor Hafiza Ismail, Nur Aqilah Mohd Razali, Rafidah Hamdan, Ahmad Fauzi Ismail
Summary: The synthesis of novel ZIF-L/GO adsorbents with different loading percentages of GO has shown high adsorption capacities for Cd(II) and confirmed the adsorption mechanism through Langmuir isotherm and pseudo-second-order kinetic model.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Nanoscience & Nanotechnology
Xiu-Shuang Xing, Xuyang Zeng, Zhongyuan Zhou, Zeinhom M. El-Bahy, Mohamed H. Helal, Qianyu Gao, Hassan Algadi, Peilin Song, Xuzhao Liu, Xinru Zhang, Jimin Du
Summary: This study presents a facile strategy to enhance the performance of photoelectrochemical water splitting using alpha-Fe2O3 photoanodes modified with metal-organic framework films doped with iron-group elements. The Co-doped MIL-125 catalyst exhibits the most excellent performance among the three dopants.
ADVANCED COMPOSITES AND HYBRID MATERIALS
(2023)
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, Multidisciplinary
Simon Krause, Jovana V. Milic
Summary: Dynamic crystalline materials combine crystalline lattice with components that display dynamic behavior in the solid state. Recent developments in this field are discussed, including the incorporation of stimuli-responsive molecular switches and machines. The opportunities and challenges associated with these materials for innovative functionality and applications are outlined.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Yuting Lei, Guihua Zhang, Qinglan Zhang, Ling Yu, Hua Li, Haili Yu, Yi He
Summary: The study demonstrates the potential application of zeolitic imidazolate frameworks as high-capacity iodine adsorbents. By using dark-field microscopy, the real-time adsorption process of gaseous I-2 on single ZIF-90 particles is visualized, revealing inter-particle heterogeneity and performance enhancement after the introduction of linker defects.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Chong Chen, Xue Li, Weixin Zou, Hui Wan, Lin Dong, Guofeng Guan
Summary: By modifying the structure of UiO-66-NH2, it was endowed with higher CO2 adsorption capacity and selectivity.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Chemical
Mengjiao Guan, Qingzhi Liu, Huiting Zhang, Qing Li, Jianan Xu, Mengmeng Cai, Weike Lin, Weina Li, Dengfeng Yang
Summary: The structure and hydrophilicity of covalent organic frameworks (COFs) can be adjusted by changing the linking group, which has a significant impact on the desalination performance of COF membranes. This study used molecular dynamics simulation to investigate the effect of different NPN-X membranes with the same elements but different linking groups on desalination performance. The results showed that NPN-1 and NPN-2 membranes exhibited superior desalination performance with much higher water permeance than conventional reverse osmosis membranes.
Article
Nanoscience & Nanotechnology
Zhenzi Yu, Dylan M. Anstine, Salah Eddine Boulfelfel, Chenkai Gu, Coray M. Colina, David S. Sholl
Summary: The study investigates various simulation methods for predicting molecule adsorption in metal-organic frameworks (MOFs), finding that adsorption-relaxation simulations are necessary for quantitative predictions in many MOFs, although standard calculations based on rigid structures can also provide useful information.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
R. Eric Sikma, Seth M. Cohen
Summary: This study reports the rational design and synthesis of three-dimensional metal-organic frameworks (MOFs) with Pd-0 and Pt-0 nodes using tetratopic phosphine ligands. Five new MOFs have been synthesized by varying the phosphine ligands and metal precursors, and they are the first examples of phosphine-metal bonded MOFs. These MOFs exhibit solid-state luminescence with significantly red-shifted emission maxima compared to Pd(PPh3)(4). Additionally, a Rh-I low-valent coordination solid based on the same linker design is reported, which displays solid-state luminescence not observed in the molecular analogue.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Inorganic & Nuclear
Jie Zhu, Laura Samperisi, Mark Kalaj, Jerika A. Chiong, Jake B. Bailey, Zhiyin Zhang, Chung-Jui Yu, R. Eric Sikma, Xiaodong Zou, Seth M. Cohen, Zhehao Huang, F. Akif Tezcan
Summary: We report the synthesis and characterization of a new series of permanently porous, three-dimensional metal-organic frameworks (MOFs), M-HAF-2 (M = Fe, Ga, or In), constructed from tetratopic, hydroxamate-based, chelating linkers. The structure of M-HAF-2 was determined by three-dimensional electron diffraction (3D ED), revealing a unique interpenetrated hcb-a net topology. This material shows high thermal and chemical stability and can be used for ionic separations.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Jessica C. Moreton, Jin Xiang Low, Katrina C. Penticoff, Seth M. Cohen, Lauren Benz
Summary: X-ray photoelectron spectroscopy can be used to compare the relative concentrations of exchanged ligands at the surface and interior regions of MOF particles, revealing the ligand distribution during PSE process. The study also found differences in surface chemistry between the PSE product and the directly synthesized product.
Article
Chemistry, Multidisciplinary
Moritz K. Jackl, Hyeonglim Seo, Johannes Karges, Mark Kalaj, Seth M. Cohen
Summary: Metalloenzyme inhibitors typically require a metal-binding pharmacophore (MBP), but MBPs can have limitations. In this study, a total of 27 salicylate metal-binding isosteres (MBIs) were synthesized as replacements for the carboxylic and hydroxyl group of the salicylic acid MBP. These salicylate MBIs were characterized for their metal-binding features, physicochemical properties, and biological activity. The results showed that salicylate MBIs can have attractive physicochemical properties and maintain or improve enzyme inhibition and selectivity.
Article
Chemistry, Organic
Johannes Karges, Seth M. Cohen
Summary: A new type of receptor molecule based on a tripodal tris(pyrrolamide) motif is presented in this study, which can bind to various anions with high affinity. The study demonstrates the ability to differentiate between enantiomeric anions through the preorganized cavity structure of the receptors.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Hyeonglim Seo, Alysia J. J. Kohlbrand, Ryjul W. W. Stokes, Jeewon Chung, Seth M. M. Cohen
Summary: Thioamides, thioureas, and thiocarbamates are introduced as stable metal-binding pharmacophores for use in metalloenzyme fragment-based drug discovery. Studies show that these molecules can act as ligands for Zn(ii)-dependent metalloenzymes including human carbonic anhydrase II and matrix metalloproteinase-2.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Medicinal
Conor B. O'Herin, Yuta W. Moriuchi, Troy A. Bemis, Alysia J. Kohlbrand, Michael D. Burkart, Seth M. Cohen
Summary: Human carbonic anhydrase II (hCAII) is a vital metalloenzyme in the human body, and its inhibitors have clinical applications in treating various diseases. This study developed degrader candidates targeting hCAII, which showed promising potential in inducing the degradation of hCAII. Optimization of the candidates resulted in a highly potent degrader with sustained depletion of hCAII. Mechanistic studies indicated that this optimized degrader functions similarly to previously reported CRBN-recruiting degraders.
JOURNAL OF MEDICINAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Johannes Karges, Miriam A. Giardini, Olivier Blacque, Brendon Woodworth, Jair L. Siqueira-Neto, Seth M. Cohen
Summary: Functionalized Re(i) tricarbonyl complexes were synthesized and found to inhibit the activity of the SARS-CoV-2 main protease, presenting a potential antiviral strategy.
Letter
Chemistry, Medicinal
Ryjul W. Stokes, Alysia J. Kohlbrand, Hyeonglim Seo, Banumathi Sankaran, Johannes Karges, Seth M. Cohen
Summary: In this study, various metal-binding isosteres (MBIs) were examined to modulate the activity of the RNA-dependent RNA polymerase acidic N-terminal (PAN) endonuclease. The inhibitory ability of MBIs against PAN was evaluated using a FRET-based enzymatic assay, and their binding mode in PAN was determined using X-ray crystallography.
ACS MEDICINAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Samuel E. Griffin, Grant P. Domecus, Clarissa E. Flores, R. Eric Sikma, Lauren Benz, Seth M. Cohen
Summary: Low-valent metal-organic frameworks (LVMOFs) and related materials have potential applications in heterogeneous catalysis, but no catalytic activity has been observed in the reported LVMOFs. In this study, a low-valent metal-organic material constructed from phosphine linkers and Ir-I nodes is reported. This material, similar to Vaska's complex, can reversibly bind O-2 and catalyze the reductive formation of enamines from amides.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Medicinal
Johannes Karges, Seth M. Cohen
Summary: Interest in covalent enzyme inhibitors as therapeutic agents has recently increased. In this article, the use of small, modular ReV complexes as inorganic cysteine-targeting warheads is described. These metal complexes were found to react rapidly and selectively with cysteine residues. The utility of these ReV complexes was demonstrated by their inhibition of SARS-CoV-2-associated cysteine proteases and human enzymes cathepsin B and L through the formation of adducts.
JOURNAL OF MEDICINAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Austin Wang, Kyle Barcus, Seth M. Cohen
Summary: The surface chemistry of three MOFs, UiO-66, MIL-88B-NH2, and ZIF-8, was investigated using dye-displacement experiments. Ligand affinity on the MOF surface was found to be dependent on the metal-ligand composition. This work provides important insights for the modulation, modification, and manipulation of MOFs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Prantik Mondal, Zhaoxi Zheng, Klaus Schmidt-Rohr, Seth M. Cohen
Summary: Postsynthetic modification (PSM) is an important tool for functionalizing metal-organic frameworks (MOFs). However, the availability of organic linkers with readily modified functional groups remains a challenge. In this study, a benzene dicarboxylic acid with azidomethyl groups was synthesized and introduced into two different MOF structures. The pendant alkyl azide groups in these MOFs were amenable to PSM via click reactions. Furthermore, the pore size restriction in one of the MOFs could be overcome by using a mixed ligand approach. Importantly, the azidomethyl groups could be reduced to primary benzylic amines, maintaining the crystallinity and porosity of the MOF.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Prantik Mondal, Seth M. Cohen
Summary: Mixed-matrix membranes (MMMs) with self-healing ability were prepared using Zr(iv)-based MOFs. These MMMs demonstrated good mechanical strength and could undergo repeated self-healing without a loss in catalytic activity towards a chemical warfare agent (CWA) simulant. The reversible hydrolysis of boronic-ester conjugates played a key role in the self-healing process.
Correction
Chemistry, Multidisciplinary
Christine N. Morrison, Kathleen E. Prosser, Ryjul W. Stokes, Anna Cordes, Nils Metzler-Nolte, Seth M. Cohen
Summary: The study introduces a novel approach using metallofragments as 3D scaffolds for fragment-based drug discovery. This method has great potential in the field of medicinal chemistry and provides a new direction for drug development.
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)
