Article
Biochemistry & Molecular Biology
Christophe Gourlaouen, Jean-Philip Piquemal
Summary: The quantum chemical nature of the Lead(II) valence basins, also known as the lead lone pair, was studied using various chemical interpretation tools including molecular orbital analysis, natural bond orbitals (NBO), natural population analysis (NPA) and electron localization function (ELF) topological analysis. The results indicate that the optimal structures of lead complexes are primarily governed by the 6s and 6p subshells, with no significant involvement of the 5d and 6d orbitals. Thus, the complexation of Pb(II) with its ligand can be explained by the interaction between the 6s(2) electrons and the accepting 6p orbitals.
Article
Multidisciplinary Sciences
O. P. de Sa Neto, H. A. S. Costa, G. A. Prataviera, M. C. de Oliveira
Summary: In this study, estimation theory is applied to a system consisting of two interacting trapped ions. A simple scheme is introduced using the Fisher matrix formalism to estimate the temperature of the longitudinal vibrational modes of the ions. The interaction between the ions is utilized to effectively infer the temperature of individual ions by optimizing the interaction time evolution and measuring only one of the ions. The effect of a non-thermal reservoir on the inference approach is also investigated.
SCIENTIFIC REPORTS
(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, Inorganic & Nuclear
Sandy Al Bacha, Sebastien Saitzek, Emma E. McCabe, Houria Kabbour
Summary: This study presents a combined experimental and computational analysis of the oxysulfide Sr6Cd2Sb6S10O7, indicating its potential for photocatalytic applications. The experimental results show efficient electron-hole separation upon visible light illumination. Density functional theory calculations and crystal orbital Hamiltonian population analysis provide insights into the electronic structure and physical properties of Sr6Cd2Sb6S10O7.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Alan M. Medina-Gonzalez, Philip Yox, Yunhua Chen, Marquix A. S. Adamson, Bryan A. Rosales, Maranny Svay, Emily A. Smith, Richard D. Schaller, Kui Wu, Aaron J. Rossini, Kirill Kovnir, Javier Vela
Summary: Alkali pnictogen dichalcogenides-I-V-VI2 are promising semiconducting materials for energy conversion devices. However, the controlled synthesis and understanding of their structures are still underdeveloped. This study successfully synthesized a series of APnCh(2) materials using solution-phase chemistry, and controlled the degree of ordering through temperature manipulation.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Ali Behjatian, Rowan Walker-Gibbons, Alexander A. Schekochihin, Madhavi Krishnan
Summary: This research investigates the long-standing issue of like-charge attraction in aqueous electrolyte, where similarly charged spheres display a minimum in their interaction potential; a proposed interfacial mechanism involving the molecular nature of the solvent explains this anomalous phenomenon; the minimum in the pair potential arises from the competition between repulsive electrostatic and solvation-induced attractive contributions.
Article
Physics, Fluids & Plasmas
J. B. Sokoloff
Summary: This paper discusses the importance of electrical image potentials in nanoscale pores, particularly in applications such as porous electrodes and nanotubes. The study found that the image potentials inside porous metallic materials are considerably larger than near flat walls, which facilitates the flow of salt ions. Additionally, the relatively large image charge potential energy in narrow nanotubes counteracts the increase in solvation energy, affecting the ion flow.
Article
Chemistry, Physical
Sandy Al Bacha, Sebastien Saitzek, Pascal Roussel, Marielle Huve, Emma E. McCabe, Houria Kabbour
Summary: This study presents the crystal structure, electronic properties, photocatalytic activity, and photocurrent response of a new antimony oxysulfide and its oxyselenide analogue. The results show promising potential for these materials in water splitting using solar energy, due to their low effective masses and strong bonding between lone pair electrons and anions.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Sang Loon Tan, See Mun Lee, Kong Mun Lo, A. Otero-de-la-Roza, Edward R. T. Tiekink
Summary: In this study, a new type of C-Cl center dot center dot center dot pi(chelate-ring) interaction in the crystal packing of an organotin dithiocarbamate compound was identified, which was shown to be attractive and possess a higher energy of association compared to other similar interactions. This adds to the variety of intermolecular interactions that can be formed by chelate-rings in the supramolecular chemistry of metal complexes.
Article
Multidisciplinary Sciences
Kasimir P. Gregory, Gareth R. Elliott, Erica J. Wanless, Grant B. Webber, Alister J. Page
Summary: The importance of ion-solvent interactions in predicting specific ion effects cannot be underestimated. However, investigations in nonaqueous systems are limited due to data deficiency. We report a database containing over 3000 simulations to study ion behavior in aqueous and non-aqueous solvent environments.
Article
Chemistry, Physical
Leandro Rezende Franco, Andre Luiz Sehnem, Antonio Martins Figueiredo Neto, Kaline Coutinho
Summary: A theoretical framework for studying ion thermodiffusion properties in aqueous solutions is proposed, using molecular dynamics simulations and ion force field parameters. The calculated single-ion properties show good agreement with experimental data, demonstrating excellent theoretical predictability. Differences in single-ion Soret and self-diffusion coefficients contribute to the thermoelectric field, quantified by the Seebeck coefficient.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Article
Chemistry, Physical
Stephen J. Cox, Kranthi K. Mandadapu, Phillip L. Geissler
Summary: Treating water as a linearly responding dielectric continuum on molecular length scales allows simple estimates of the solvation structure, but computer simulations show quantitative inaccuracies and an inability to capture certain aspects of microscopic polarization response. By modifying the dielectric continuum model based on physical inspiration and analyzing the orientational response of water molecules, a field theory with suggested form is proposed to break the charge symmetry of ion solvation and provide solvation free energies that closely match simulation results.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Agriculture, Multidisciplinary
Nicholas Jarvis, Mats Larsbo, Elisabet Lewan, Sarah Garre
Summary: Accurate modeling of hydrological processes in the soil-crop system is crucial for assessing the impacts of soil management and climate change. The use of empirical treatments in water flow processes limits the applicability and increases prediction errors in crop models. Physics-based descriptions are available, but their significance is often overlooked.
AGRICULTURAL SYSTEMS
(2022)
Article
Chemistry, Multidisciplinary
Martina Havlikova, Adam Jugl, Jitka Krouska, Jana Szabova, Ludmila Mravcova, Tereza Venerova, Chien-Hsiang Chang, Miloslav Pekar, Filip Mravec
Summary: High-resolution ultrasound spectroscopy, size and zeta-potential titrations, and isothermal titration calorimetry were used to characterize the interactions between hyaluronan and catanionic ion pair amphiphile vesicles. The interactions showed a correlation between data from size titration, HR-US, and visual observation. Intensity of interactions and the disaggregation were dependent on the molecular weight of hyaluronan.
Article
Chemistry, Multidisciplinary
Jing Liu, Dengpan Dong, Alan Larrea Caro, Nicolai Sage Andreas, Zongjian Li, Yunan Qin, Dimitry Bedrov, Tao Gao
Summary: This study reports a novel Fe electrolyte that significantly improves the Coulombic efficiency and cycling performance of Fe metal batteries by adding magnesium ions or calcium ions, and the mechanism for the improved efficiency is elucidated.
ACS CENTRAL SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Mengsu Peng, Timothy T. Duignan, Cuong Nguyen, Anh Nguyen
Summary: Surfactants play a central role in various scientific and engineering fields, but understanding their behavior at the air-water interface still presents challenges. Research focuses on accurately describing the adsorption layer thickness of surfactants in this area. The modified Poisson-Boltzmann model has been developed to address the effects of surfactants at the air-water interface, with remaining challenges and future research directions also discussed.
Article
Chemistry, Physical
Timothy T. Duignan
Summary: This study investigates the mechanism of ions preventing bubble coalescence in water, finding that the Gibbs-Marangoni pressure explains this phenomenon, and the distribution of ions and surface potential affect this pressure, thereby impacting the ability of bubble coalescence.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Chemistry, Physical
Ayman E. Elkholy, Timothy T. Duignan, Xiaoming Sun, Xiu Song Zhao
Summary: This study demonstrates that an alpha-MoO3 electrode prepared using the electrochemical deposition method exhibits stability in neutral aqueous electrolytes and a wide potential window, attributed to enhanced electron conductivity and dense microstructure. The widened potential window is linked to the electrocatalytic inactivity of alpha-MoO3 towards water electrolysis and high overpotentials of the neutral electrolyte for H-2 and O-2 evolution reactions.
ACS APPLIED ENERGY MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Timothy T. Duignan, Shawn M. Kathmann, Gregory K. Schenter, Christopher J. Mundy
Summary: This article emphasizes the significance of using quantum mechanics based first-principles interaction potentials to enhance the understanding of electrolyte solutions, with a focus on quantum density functional theory combined with molecular dynamics simulation. The balance between local structure and long-range correlations is crucial for predicting thermodynamics of single ions and collective interactions.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Physical
Dedi Wang, Renjie Zhao, John D. Weeks, Pratyush Tiwary
Summary: By studying NaCl ion-pair dissociation in a dilute aqueous solution using computer simulations, we find that short-range interactions can accurately reproduce the dissociation process, while contributions from long-range interactions can be neglected.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Cuong Nguyen, Mengsu Peng, Timothy T. Duignan, Anh Nguyen
Summary: The impact of salt ions on the adsorption of surfactants at the air-water interface was investigated. It was found that the size and charge of the ions play a critical role in the adsorption process.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Electrochemistry
Ayman E. Elkholy, Timothy T. Duignan, Tanveer Hussain, Ruth Knibbe, Xiu Song Zhao
Summary: This paper investigates the influence of charge density of the studied aqueous electrolyte cations (Na+, Mg2+, and Al3+) on the electrochemical performance of the alpha-MoO3 electrode. It reveals that the charge storage capacity increases with increasing cation charge density, while the initial coulombic efficiency decreases and the charge transport kinetics are slowed down. This study provides valuable insights into the relationship between metal ion charge density and their electrochemical behavior towards the alpha-MoO3 electrode in aqueous solutions and emphasizes the importance of selecting appropriate aqueous electrolytes to enhance electrochemical performance.
Article
Electrochemistry
Ayman E. Elkholy, Timothy T. Duignan, Ruth Knibbe, Xiu Song Zhao
Summary: This study reports on a polypyrrole-encapsulated alpha-MoO3 electrode with high cycling stability and high rate capability for aqueous electrochemical energy storage.
ELECTROCHIMICA ACTA
(2022)
Review
Chemistry, Physical
Mike Tebyetekerwa, Timothy T. Duignan, Zhen Xu, Xiu Song Zhao
Summary: This article provides an overview of the development, electrochemistry, and challenges of dual-carbon batteries (DCBs). It summarizes past lessons in ion intercalation and addresses current issues affecting DCBs, along with potential remedies. The article also highlights the importance of significant research efforts in advancing the commercialization and adoption of DCBs for a sustainable and circular economy.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Ang Gao, Richard C. Remsing, John D. Weeks
Summary: In this article, recent developments in the local molecular field (LMF) theory are reviewed, which addresses the challenges of Coulomb interactions in aqueous solutions. LMF theory accurately separates intermolecular Coulomb interactions into short-range and long-range components, reducing the need for complex lattice summation techniques. The short solvent (SS) model, derived from LMF theory, provides a simple description of the pairing of nucleobases and biologically relevant ions in water.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Nanoscience & Nanotechnology
Mohamed Nazmi Idros, Yuming Wu, Timothy Duignan, Mengran Li, Hayden Cartmill, Irving Maglaya, Thomas Burdyny, Geoff Wang, Thomas E. Rufford
Summary: This study explores the effects of solvent-ionomer interactions on the structure and performance of Cu catalyst layers (CLs) for CO2 electrolysis. The findings suggest that using acetone as the dispersion solvent can lead to better performance and higher selectivity, with acetone-CL exhibiting a 25% higher selectivity for C2+ products compared to methanol-CL at high current density.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Sophie Baker, Joshua Pagotto, Timothy T. Duignan, Alister J. Page
Summary: Neural network potentials have proven to be an efficient tool for accelerating ab initio molecular dynamics simulations. This study explores the use of existing DFTB molecular dynamics data to train graph neural network potentials and accurately reproduce solvation structures in NaCl solutions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
R. M. N. M. Rathnayake, Debra J. Searles, Timothy T. Duignan, X. S. Zhao
Summary: Diglyme co-intercalation with sodium ion into graphite can potentially be used as an anode for sodium-ion batteries. The functionalisation of diglyme molecules with fluoro and hydroxy groups significantly affects the binding between sodium, the solvent ligand, and graphite. The hydroxy-functionalised diglyme exhibits the strongest binding to graphite and the graphene layer enhances the binding of the sodium-diglyme complex to the graphene layer.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Applied
Ayman E. Elkholy, Timothy T. Duignan, Ruth Knibbe, Xiu Song Zhao
Summary: The charge-storage performance of orthorhombic molybdenum trioxide (a-MoO3) electrode material was investigated in two different electrolytes. It was found that a-MoO3 electrode exhibited poor cycling stability in the electrolyte based on aluminium trifluoromethanesulfonate (Al(OTf)3)-water solution, but showed significantly improved stability in the water-in-salt electrolyte (WiSE). The difference in cycling stability was attributed to the maintenance of the crystal structure in WiSE and the substantial structural degradation in the Al(OTf)3-based salt-in-water electrolyte (SiWE).
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Chemistry, Physical
Junji Zhang, Joshua Pagotto, Timothy T. Duignan
Summary: Electrolyte solutions are crucial in materials chemistry applications, but determining their properties from first principles remains challenging. Recent advances in deep learning, particularly equivariant neural network potentials, offer a potential solution by accelerating sampling of electrolyte solution configurations.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)