Article
Chemistry, Multidisciplinary
Takakazu Seki, Chun-Chieh Yu, Kuo-Yang Chiang, Alessandro Greco, Xiaoqing Yu, Fumiki Matsumura, Mischa Bonn, Yuki Nagata
Summary: In typical aqueous systems, multiple ion species are co-solvated, and these ions at the water-air interface can have significant impacts on chemical reactivity, aerosol formation, climate, and water odor. Through sum-frequency generation spectroscopy, researchers have quantified the relative surface activity of two co-solvated ions and found that hydrophobic ions tend to be speciated to the water interface due to the presence of hydrophilic ions. The speciation of ions at electrolyte solution interfaces is determined by the solvation energy difference between the ions and the intrinsic surface propensity of ions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Shahrazad M. A. Malek, Victor Kwan, Ivan Saika-Voivod, Styliani Consta
Summary: The interactions between water and ions within droplets are critical in the chemical reactivity of atmospheric and man-made aerosols. Computational evidence shows that in supercooled aqueous nanodroplets, a lower density core of tetrahedrally coordinated water expels ions to the denser subsurface. At room temperature, the radial distribution in the droplet core varies depending on the ion's nature.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Xiaohu Yang, Hanqing Gu, Qiwen Sun, Wenming Zhang, Zhanyu Li
Summary: As a promising competitor for large-scale energy storage components in the future, aluminum batteries have gained attention. However, the sensitivity to air and corrosiveness of nonaqueous electrolytes hinder the development of aluminum ion batteries. Aluminum batteries meet the needs of green development and are a key research focus.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Physical
Junyi Yin, Mingyan Li, Xiang Feng, Tianyi Cui, Weiyu Sun, Minghui Wang, Weichen Shi, Shujiang Ding, Yonghong Cheng, Xin Xu, Jianhua Wang
Summary: Caprolactam shows great potential as an electrolyte additive for achieving stable and reliable zinc-based batteries by enhancing the reversible deposition of zinc anodes and optimizing the solvation structures.
JOURNAL OF ALLOYS AND COMPOUNDS
(2024)
Article
Engineering, Environmental
Xin Xu, Xiang Feng, Mingyan Li, Junyi Yin, Fuxiang Li, Jingzhe Chen, Weichen Shi, Yonghong Cheng, Jianhua Wang
Summary: The issue of dendrites in neutral/mild electrolyte-based aqueous zinc-ion batteries has been a problem for a long time. The enhanced electrostatic shielding effect of a hybrid additive of Na2SO4 and EDTA is utilized to induce uniform Zn deposition and suppress the growth of Zn dendrites. The coordination of EDTA provides a more stable solvation shell for Na+ and ensures a stronger blocking effect on Zn deposition at the tip, leading to improved cycle life of the battery.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Viktor Rozsa, Giulia Galli
Summary: The interaction between ions and water at high pressure and temperature has significant effects on geochemical properties. However, the average structural and vibrational properties of water are weakly affected by ions at extreme conditions, and the presence of ions only slightly increases the ionic conductivity of the liquid and moderately reduces the dielectric constant.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Engineering, Environmental
Mahsa Khajeh, Mohammad Mehdi Amin, Ali Fatehizadeh, Tejraj M. Aminabhavi
Summary: The research investigated the removal of atenolol from aqueous solutions using hydrodynamic cavitation and sodium persulfate as a zero-waste discharge process. The study showed that pH, coexisting anions, and reaction time significantly affected the efficiency of atenolol removal. The HC-PS process was proven to be effective in degrading pharmaceutical pollutants from water and wastewater sources.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Trenton C. Gallagher, Che-Yu Wu, Marcos Lucero, Sean K. Sandstrom, Lindsey Hagglund, Heng Jiang, William Stickle, Zhenxing Feng, Xiulei Ji
Summary: This study reports a dual-ion battery using copper as an electrode for carbonate conversion reactions, which can be used for CO2 consumption and storage. The copper electrode exhibits reversible capacity and relatively stable cycling performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Qianyi Ma, Rui Gao, Yizhou Liu, Haozhen Dou, Yun Zheng, Tyler Or, Leixin Yang, Qingying Li, Qiao Cu, Renfei Feng, Zhen Zhang, Yihang Nie, Bohua Ren, Dan Luo, Xin Wang, Aiping Yu, Zhongwei Chen
Summary: The addition of 2-propanol is shown to regulate the outer solvation shell structure of Zn2+ in aqueous Zn-ion batteries, resulting in uniform Zn deposition and dendrite-free growth.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Yanxin Shang, Shi Chen, Nan Chen, Yuejiao Li, Jingning Lai, Yue Ma, Jun Chen, Feng Wu, Renjie Chen
Summary: Aqueous batteries are gaining attention for their safety and low cost. However, their narrow electrochemical stability window and limited working temperature range have posed challenges. This study introduces a new solvent that can break the water hydrogen bond network and enhance the stability of the electrolyte, resulting in a wider stability window and lower freezing point. The electrolyte also demonstrates good cycling performance at high temperatures.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Rabi Khanal, Stephan Irle
Summary: Quantum chemical molecular dynamics simulations were used to investigate the impact of K+, Na+, and Mg2+ ions on the static and dynamic structure of bulk water in aqueous solutions. The study found that salt ions generally slow down the dynamic decay of pair correlations in the water solvation sphere, with differences observed between different cation types.
Article
Chemistry, Physical
Jan Thogersen, Tobias Weidner, Frank Jensen
Summary: The primary photolysis dynamics of aqueous carbonate and hydrogen carbonate when excited at lambda = 200 nm were studied using UV pump-Vis probe and UV pump-IR probe transient absorption spectroscopy and density functional theory calculations. The dissociation and electron detachment processes were observed, as well as the assistance of water molecules in the dissociation of CO32-. The primary photolysis of hydrogen carbonate was obscured by the photo-products of carbonate, but the two-photon ionization of water allowed for the study of aqueous carbonic acid.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Electrochemistry
Shi-You Li, Fei Xu, Ning-Shuang Zhang, Peng Wang, Jie Wang
Summary: This study illustrates the specific role of lithium salt anions in the SEI film formation process by comparing their influence on solvation structure with two kinds of boron containing lithium salts. The findings show that lithium salt anions can impact the coordination capability of lithium ions and solvents, influencing the energy consumption in the desolvation process of lithium ions and the composition of SEI film.
BATTERIES & SUPERCAPS
(2022)
Article
Chemistry, Multidisciplinary
Darren M. Driscoll, Sydney N. Lavan, Milena Zorko, Paul C. Redfern, Stefan Ilic, Garvit Agarwal, Timothy T. Fister, Rajeev S. Assary, Lei Cheng, Dusan Strmcnik, Mahalingam Balasubramanian, Justin G. Connell
Summary: As the search for new battery chemistries expands, understanding and controlling the working cation solvation structure is key to enabling improved stability and reversibility. In this work, an emergent solvation behavior is discovered in multivalent electrolytes, allowing for the modification of electrochemical response and activating additional redox species. This suggests a new framework for electrolyte design, enabling profound changes to the electrochemical behavior of the system.
Article
Chemistry, Physical
Ke Li, Visal Subasinghege Don, Chris S. Gupta, Rolf David, Revati Kumar
Summary: The differences in ion association and charge transport between NaOTf and NaTFSI at different salt concentrations in glymes with increasing chain length were studied using molecular simulations. The results showed similar trends in ion association behavior as a function of salt concentration for both NaOTf and NaTFSI, but the dominant solvation structures were distinctly different in different glyme concentrations. Conductivity was affected by ion association behavior and non-vehicular transport of anions in these electrolytes systems.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Tarek Marei, Mahmoud K. Al-Joumhawy, Mohammad A. Alnajjar, Werner M. Nau, Khaleel Assaf, Detlef Gabel
Summary: A new set of hybrid guest molecules bearing organic and inorganic residues have been studied for their recognition properties by cyclodextrins in aqueous solution. The results show that they exhibit sizable affinity to cyclodextrins and unexpected photophysical properties.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Foad N. Tehrani, Khaleel Assaf, Robert Hein, Casper M. E. Jensen, Thomas C. Nugent, Werner M. Nau
Summary: Compared to Diels-Alder reactions involving heteroatom-containing substrates, the endo dimerization of cyclopentadiene is minimally affected by changes in the microenvironment or the presence of potential catalysts. It has been observed that the intermediate-sized cucurbit[7]uril can selectively and efficiently catalyze this reaction in aqueous solution, while other macrocyclic homologues have no acceleration or inhibitory effect. The addition of methanol can overcome the expected product inhibition and achieve high catalytic turnover numbers.
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)
