Review
Chemistry, Multidisciplinary
Jane Arciszewski, Karine Auclair
Summary: Mechanoenzymology is an emerging field that utilizes mechanical mixing to sustain enzymatic reactions in low-solvent or solvent-free mixtures. It can be applied to the synthesis or depolymerization of polymeric materials, offering various advantages.
Article
Chemistry, Multidisciplinary
Antonio Bauza, Antonio Frontera
Summary: In this study, we propose the term Wolfium bond (WfB) to describe the net attractive force between group 6 elements and electron donor atoms. By analyzing the X-ray crystal structures of proteins and conducting ab initio calculations, we provide evidence for the existence of this interaction and explore its potential biological role and physical nature.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Review
Chemistry, Multidisciplinary
Si-Qi Chen, Wei Zhao, Biao Wu
Summary: The proper concentration of sulfate anion is essential for key physiological functions, and recent research on sulfate recognition and separation has made progress, with molecular recognition being the key element for selective sulfate separations.
FRONTIERS IN CHEMISTRY
(2022)
Article
Chemistry, Physical
Laicheng Zhou, Ran He, Yang Qin, Yi-Lin Wu, Li Jiang, Dong-Dong Zhou, Ling Zhang
Summary: In this study, a strategy for directed self-assembly based on C-H/N-H...anion hydrogen bond enhanced pi-pi interactions in water was reported, allowing for precise control of surface charge distance in nanosheets, with potential applications in capturing DNA.
Article
Chemistry, Inorganic & Nuclear
Margarita Bulatova, Daniil M. Ivanov, J. Mikko Rautiainen, Mikhail A. Kinzhalov, Khai-Nghi Truong, Manu Lahtinen, Matti Haukka
Summary: This study found rare halogen bonding with metal-involved stabilizing contact in two metallopolymeric cocrystals, and investigated the nature of their noncovalent contact. Computational studies revealed that the I...I halogen bond is the strongest noncovalent interaction in both systems.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Saurav Bhattacharya, Andrea Barba-Bon, Tsedenia A. Zewdie, Anja B. Mueller, Talha Nisar, Anna Chmielnicka, Iwona A. Rutkowska, Christian J. Schuermann, Veit Wagner, Nikolai Kuhnert, Pawel J. Kulesza, Werner M. Nau, Ulrich Kortz
Summary: We report the discovery of the first two cationic palladium(II)-oxo clusters (POCs) containing f-metal ions, and investigate their physicochemical characterization. The molecular structure of these novel POCs consists of an octahedral {Pd6O12} core capped by eight M-IV ions, forming a cationic, cubic assembly {Pd6O12M8IV}. We also found that these POCs can form host-guest inclusion complexes with 4-sulfocalix[n]arenes, and can be used as pre-catalysts for electrocatalytic CO2 reduction and HCOOH oxidation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Bohuai Xiao, Suhang He, Mingjun Sun, Jianghao Zhou, Zhiye Wang, Yunchuan Li, Simin Liu, Werner M. Nau, Shuai Chang
Summary: This study introduces a versatile recognition tunneling technique using doubly cucurbit[7]uril-functionalized electrodes to form supramolecular junctions that capture analytes dynamically by host-guest complexation, resulting in characteristic changes in their single-molecule conductance. For structurally related drug molecules and mixtures, distinct current switching signals related to their intrinsic conductance properties and pH-dependent effects are observed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
Andrea Barba-Bon, Giulia Salluce, Irene Lostale-Seijo, Khaleel Assaf, Andreas Hennig, Javier Montenegro, Werner M. Nau
Summary: This study demonstrates that globular dodecaborate clusters can function as anionic inorganic membrane carriers for a wide range of hydrophilic cargo molecules. These carriers have the potential to transport peptides, amino acids, neurotransmitters, vitamins, antibiotics, and drugs across liposomal membranes, and affect the cytosolic uptake of various small bioactive molecules.
Article
Chemistry, Multidisciplinary
Mohamed Nilam, Shreya Karmacharya, Werner M. Nau, Andreas Hennig
Summary: This study demonstrates a significant increase in sensitivity of supramolecular chemosensors by encapsulating them inside liposomes and exposing them to a pH gradient. The enhanced sensors can effectively detect multiple biologically relevant analytes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biology
Muriel Masi, Julia Vergalli, Ishan Ghai, Andrea Barba-Bon, Therese Schembri, Werner M. Nau, Daniel Lafitte, Mathias Winterhalter, Jean-Marie Pages
Summary: This study investigated the translocation and killing effects of different cephalosporins on Gram-negative bacteria. The results revealed that the activity and efficiency of the drugs were influenced by the expression of specific porins. Through experimentation and analysis, it was found that the net negative charge of one of the cephalosporins contributed to its higher permeation through less cation-selective porins. These findings provide insights into the susceptibility of specific bacteria strains to cephalosporins.
COMMUNICATIONS BIOLOGY
(2022)
Article
Agriculture, Multidisciplinary
Francisco J. R. Mejias, Suhang He, Rosa M. Varela, Jose M. G. Molinillo, Andrea Barba-Bon, Werner M. Nau, Francisco A. Macias
Summary: This paper presents a solution to the limited application of aminophenoxazinones and their sulfur mimics in agriculture, by utilizing host-guest complexation with cucurbiturils (CBn). Research shows that CB7 is the most suitable homologue due to its strong affinity for guest molecules and high water solubility. The formation of complexes was studied through direct titrations and UV-vis spectroscopy, showing preferential interaction with protonated aminophenoxazinone species. NMR characterization and stability analysis revealed pK(a) modulation and stabilization by cucurbiturils, enhancing the bioactivity of APO and DiS-NH2.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2023)
Article
Chemistry, Organic
Jinling Zhang, Detlef Gabel, Khaleel I. Assaf, Werner M. Nau
Summary: This study investigates the binding interaction between perhalogenated boron clusters derived from B12Br122- and cyclodextrins, finding high binding affinity in aqueous solution. A novel fluorescein-substituted perbrominated dodecaborate cluster is synthesized through a copper(I)-catalyzed azide-alkyne click reaction. The formation of inclusion complexes between the cluster-modified dye and cyclodextrins is easily tracked through optical titrations.
Article
Polymer Science
Maik H. H. Jacob, Roy N. N. D'Souza, Alexandra I. I. Lazar, Werner M. M. Nau
Summary: In the field of polymer structure and dynamics, fluorescence spectroscopy may provide answers to questions that cannot be solved by AI, X-ray, or NMR techniques. FRET theory describes how optically excited fluorophores transfer their energy to an acceptor moiety, depending on the distance between donor and acceptor. However, the dependence on distance distribution and diffusion is described by a partial differential equation (HSE) that can only be solved numerically. Time-resolved measurements and global analysis of extensive data sets are required. The Haas-Steinberg-Jacob equation (HSJE) provides a closed analytical expression and allows for faster and more accurate analysis.
Article
Chemistry, Multidisciplinary
Suresh Moorthy, Hugues Lambert, Neetha Mohan, Thomas Schwarzlose, Werner. M. M. Nau, Elina Kalenius, Tung-Chun Lee
Summary: In the gas phase, thermal activation of supramolecular assemblies commonly leads to noncovalent dissociation, but exceptions exist for certain chemical reactions within host-guest complexes. Mass spectrometry revealed that the complexation of 1-amino-methyl-2,3-diazabicyclo[2.2.2]oct-2-ene (DBOA) by β-cyclodextrin resulted in collision-induced dissociation, while complexation by cucurbit[7]uril (CB7) led to competitive chemical reactions upon thermal activation. These findings demonstrate that noncovalent interactions can direct chemical reactions in the gas phase.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Materials Science, Multidisciplinary
Matias Paatelainen, Markus Lahikainen, Alex Berdin, Kim Kuntze, Werner M. Nau, Nonappa, Arri Priimagi
Summary: Supramolecular host-guest complexes are dynamic systems consisting of macrocyclic host molecules encapsulating smaller guest molecules, and can be used to tackle fluorescence quenching and photobleaching. This study demonstrates the application of supramolecular host-guest complexation in a hydrogel network to create tunable hydrogel-based lasers. By doping hydrogel with cucurbit[7]uril as a host molecule, the fluorescent quantum yield and photostability of Rhodamine B molecules in the hydrogel are significantly improved. A thin-film distributed feedback hydrogel laser with wavelength tunability is fabricated to showcase the concept. These findings, combined with the stimuli-response of hydrogels, open up possibilities for affordable and small-scale photonic devices for sensing applications.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Katie McGuire, Suhang He, Jennifer Gracie, Charlotte Bryson, Dazhong Zheng, Alasdair W. Clark, Jesko Koehnke, David J. France, Werner M. Nau, Tung-Chun Lee, William J. Peveler
Summary: This study demonstrates that aggregation of fluorescent quantum dot (QD) linked with cucurbiturils (CBs) can be broken-up by including guest molecules, while retaining CBs adsorbed on the surface. At the same time, the QD surface can be modified by the functional tail of the guest, enabling a non-covalent, click-like modification of nanoparticles in aqueous solution. This approach provides divergent routes for nano-architectures with rich functionalities for theranostics and photonics in aqueous systems.
Article
Chemistry, Multidisciplinary
Suhang He, Bing Huang, Bohuai Xiao, Shuai Chang, Marina Podalko, Werner M. Nau
Summary: Docking of alkali metal ions to water-soluble macrocyclic receptors can unexpectedly enhance the binding of guest molecules. For example, with cucurbit[5]uril and large cations, methane and ethane binding increased 5-8 times due to water molecule removal during cation binding. This reveals a previously unnoticed steric hindrance of solvation water molecules near receptor binding sites.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Organic
Khaleel I. Assaf, Werner M. Nau
Summary: Large water-soluble anions with chaotropic character exhibit strong supramolecular interactions in water with macrocyclic receptors, polymers, biomembranes, and hydrophobic cavities/interfaces. The driving force behind this high affinity, the chaotropic effect, is orthogonal to the common hydrophobic effect. This review focuses on the binding of large anions to water-soluble macrocyclic hosts, highlighting their applications in various fields.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Khaleel I. Assaf, Werner M. Nau
Summary: In the past decade, there has been significant progress in understanding the importance of London dispersion interactions (LDIs) in supramolecular systems and solutions. It has been found that arguments related to molecular polarizabilities, which are often used to explain intermolecular interactions, may not always apply to the condensed phase. Therefore, when studying association phenomena in solutions, it is recommended to use bulk polarizabilities, which can be determined experimentally. CBn compounds are privileged molecular container compounds that can be used to study the binding of hydrophobic molecules and the influence of LDIs on chemical reactions.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Agriculture, Multidisciplinary
Francisco J. R. Mejias, Suhang He, Rosa M. Varela, Jose M. G. Molinillo, Andrea Barba-Bon, Werner M. Nau, Francisco A. Macias
Summary: This paper presents a solution to the limited application of aminophenoxazinones and their sulfur mimics in agriculture by using host-guest complexation with cucurbiturils (CBn). The most suitable CBn homologue was found to be CB7 due to its strong affinity for guest molecules and high water solubility. The complex formation between CB7 and aminophenoxazinones was studied and shown to have high binding affinities and improved stability and bioactivity.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2022)
Article
Chemistry, Organic
Faiza Diaba, Gisela Trenchs
Summary: The first violet light-mediated synthesis of gamma- and delta-lactams from N-alkenyl trichloroacetamides is reported in this paper. The reactions are conducted in tetrahydrofuran or 2-methyltetrahydrofuran as the sole solvent without catalysts or additives, under non-anhydrous conditions in an air atmosphere where the solvent serves as the radical initiator.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Article
Chemistry, Organic
Feroze Hussain, Sajjad Ahmed, Ashiq Hussain Padder, Qazi Naveed Ahmed
Summary: This study reports a novel and efficient one-pot synthesis method for mixed phosphorotrithioates, which does not require supplementary additives and shows broad applicability.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Article
Chemistry, Organic
Hyunjin Oh, Ikyon Kim
Summary: A new 1,2,4-triazole-pyrrolo[1,2-a]pyrazine hybrid system, 6-acylpyrrolo[1,2-a][1,2,4]triazolo[5,1-c]pyrazine, was synthesized using a catalyst-free method. This method involved sequential exposure of pyrrole-2-carbonitrile-derived substrates to DMF-DMA and acyl hydrazide, resulting in the formation of acylated pyrazine and 1,2,4-triazole rings, enabling the installation of various substituents at specific positions on the core skeleton.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Article
Chemistry, Organic
Ming Yan, Si-fan Wang, Yong-po Zhang, Jin-zhong Zhao, Zhuo Tang, Guang-xun Li
Summary: Here we developed an efficient photocatalytic approach for the convenient preparation of sulfinamides. The reaction allows for the gram-scale preparation of sulfinamides and the one-pot synthesis of various sulfonyl amides.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Article
Chemistry, Organic
Farzaneh Bandehali-Naeini, Zahra Tanbakouchian, Noushin Farajinia-Lehi, Nicolas Mayer, Morteza Shiri, Martin Breugst
Summary: Two tandem catalytic systems were developed for the synthesis of novel 3,4-disubstituted maleimides using the same Ugi adducts. Different maleimide structures can be synthesized using either Pd or Cu catalysis.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Article
Chemistry, Organic
Tanya Raghava, Anjan Chattopadhyay, Subhadeep Banerjee, Nivedita Sarkar
Summary: Amine substitution of two ortho fluorine atoms of tetrafluoroterephthalonitrile through SNAr chemistry is easily achievable. But further fluorine substitution is only possible under forcing conditions, yielding valuable fluorophores for bioimaging.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)
Review
Chemistry, Organic
Anju Chadha, Santosh Kumar Padhi, Selvaraj Stella, Sowmyalakshmi Venkataraman, Thangavelu Saravanan
Summary: Alcohol dehydrogenases are enzymes that use cofactors for oxidation or reduction reactions of alcohols or carbonyl compounds. They are utilized in green chemistry and have applications in the production of pharmaceuticals. Recombinant enzymes have solved the challenge of producing purified enzymes in large quantities. Engineered alcohol dehydrogenases have been used in asymmetric synthesis in industry. Various methods have been established for regenerating expensive cofactors to make the enzymatic process more efficient and economically viable.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2024)