Article
Chemistry, Physical
Rhys P. King, William Levason, Gillian Reid
Summary: The tetra-alkylammonium tetrathioantimonate(V) salts were prepared and characterized. The alkylammonium salts showed solubility in water and weakly polar organic solvents, and [N(n-Bu)4]3[SbS4] was found to be suitable for studying coordination chemistry or materials applications that cannot use water as a solvent. Furthermore, a thiosulfate complex of a p-block element was obtained through the decomposition of [N(n-Bu)4]3[SbS4] in acidic media.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Physical
Riya Bag, Yeasin Sikdar, Sutapa Sahu, Jayanta Bag, Michael G. B. Drew, Kuntal Pal, Sanchita Goswami
Summary: This study presents new chemosensors capable of selectively detecting F- and Hg2+ in the micromolar range. Modulating proton acidity by introducing an electron donating group in the probe backbone affects sensing outcomes. The mechanism of sensing of the analytes is supported by detailed DFT and TD-DFT analyses.
Article
Chemistry, Physical
Jakub Brzeski, Sylwia Freza, Marcin Czapla, Piotr Skurski
Summary: The study investigated the stable anionic states formed by Grignard reagents compared to magnesium halides, finding that Grignard compounds form stable valence-bound systems with significant electron detachment energies. Additionally, structural relaxation was predicted for Grignard compounds when an extra electron is attached.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Inorganic & Nuclear
Erika Stefano, Federica De Castro, Erik De Luca, Antonella Muscella, Santo Marsigliante, Michele Benedetti, Francesco P. Fanizzi
Summary: A new series of complexes were synthesized and their cytotoxicity on cancer cells was studied. Among them, the 2b complex with a longer alkyl chain showed higher cytotoxicity in certain cancer cell lines.
INORGANICA CHIMICA ACTA
(2023)
Article
Chemistry, Physical
Anne S. Hansen, Rachel M. Huchmala, Emil Vogt, Mark A. Boyer, Trisha Bhagde, Michael F. Vansco, Casper V. Jensen, Alexander Kjaersgaard, Henrik G. Kjaergaard, Anne B. McCoy, Marsha I. Lester
Summary: The study reveals a strong coupling between the OH-stretch and torsion vibrations in tert-butyl hydroperoxide, leading to a double well potential associated with torsional motion. Experimental results show that theoretical models incorporating this coupling are necessary to explain the spectral features observed in the first OH-stretching overtone region of TBHP. Comparing theory and experiment highlights the importance of including OH-stretch and COOH torsion treatments in order to unravel the observed features.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Katsuumi Nagai, Hisashi Honda
Summary: Four new ionic rotator-crystals were observed, with large degrees of motion for both cations and anions. Measurements using nuclear magnetic resonance and differential scanning calorimetry revealed the rotation and reorientation behaviors of the crystals in the solid phase.
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION A-A JOURNAL OF PHYSICAL SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Robert D. Riley, Katherine N. Robertson, Jason A. C. Clyburne
Summary: The reaction between bis(dialkylphosphino)amines and elemental halogens produces cationic products. Some of these compounds can react further with methanol to produce salts.
CANADIAN JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Bao Chen, Chuan-Hui Zhang, Ying Jin
Summary: This study systematically investigated the roles of Cl- and OH- in the dissociation of H2O on an Al surface through first-principles calculations. Different co-adsorption models were designed and the conditions for OH--induced H2O dissociation were discussed. The catalytic role of Cl- in the H2O dissociation process on an Al surface was proposed based on electronic structure analysis.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2021)
Article
Materials Science, Multidisciplinary
Shi-Yu Ma, Jin-Kai Li, Zong-Ming Liu
Summary: Inorganic halide perovskite quantum dots show excellent optical and photoelectric properties, but their commercial application is hindered by instability. This study introduces a PbX (OH) (X = Cl,Br) encapsulation layer to improve the stability of CsPbX3 (X = Cl,Br) perovskite quantum dots in polar solvents. The encapsulation layer acts as a water-blocking and protective layer, reducing surface passivation and trap density, and greatly enhancing the photoluminescence quantum yield and stability of the perovskite structure.
Article
Chemistry, Physical
Jianchuan Liu, Renxi Liu, Yu Cao, Mohan Chen
Summary: This study uses the deep potential molecular dynamics (DPMD) method to simulate the solvation structures of calcium (Ca2+) and magnesium (Mg2+) ions with hydroxide (OH-) ion in water. The study provides new insights into the differences in the solvation structures of Ca2+ and Mg2+ ions in the presence of OH-, showing that OH- has a more significant effect on the solvation structure of Ca2+ compared to Mg2+. In addition, the study reveals the changes in the solvation structure of OH- in the presence of the cations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Inorganic & Nuclear
Marjaana Taimisto, Tom Bajorek, J. Mikko Rautiainen, Tapani A. Pakkanen, Raija Oilunkaniemi, Risto S. Laitinen
Summary: The pathways to the formation of a series of [RuCl2(CO)(2)(ERR ')(2)] complexes have been explored experimentally and computationally. The results show that the reaction rate is faster in THF and the highest yield is observed for the telluroether complexes. The nature of the solvent does not affect the reaction path. The substitution of one CO ligand by the second ERR ' is the rate-determining step. The formation of [RuCl2(CO)(3)(THF)] is observed in THF, but it is not necessary for the dissociation of [RuCl2(CO)(3)](2).
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
I. Alkorta, A. C. Legon
Summary: In this study, equilibrium dissociation energies of halogen- and hydrogen-bonded complexes were calculated and the electrophilicities of various Lewis acids were determined. The ratios of electrophilicities for different Lewis acids were found to be independent of the type of non-covalent interaction involved. Additionally, molecular electrostatic surface potentials showed a strong correlation between dissociation energies and maximum positive electrostatic potentials.
Article
Chemistry, Multidisciplinary
Yee Seng Tan, Chien Ing Yeo, Huey Chong Kwong, Edward R. T. Tiekink
Summary: Linear coordination polymers with one-dimensional structures have been fully characterized using various techniques. The crystal structures and supramolecular associations were found to be influenced by different substituents.
Article
Chemistry, Organic
Mathieu Morency, Sebastien Neron, Radu Iftimie, James D. Wuest
Summary: This study established a simple method based on a linear relationship to predict pK(a) values of quinonoid compounds, with high accuracy for handling complex analogues with multiple OH groups and intramolecular hydrogen bonds. The approach allows reliable predictions of acidity, selection of proper pK(a) values, and determination of deprotonation sites and orders in complex structures.
JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Inorganic & Nuclear
Simon Thomas, James P. Ward, Jonathan M. White, Charles G. Young
Summary: The reaction of Tp*(WI)-I-II(CO)(2) with (R)-( + )-alpha-methylbenzylamine in dichloromethane produces blue, diamagnetic Tp*W-II(R)-(+)-LHI(CO)(2). This complex features a six-coordinate, distorted-octahedral structure and is unusually stable and resistant to oxygen- and sulfuratom transfer reactions.
INORGANICA CHIMICA ACTA
(2021)
Article
Chemistry, Physical
Wenjie Yan, Xin Xu
Summary: An analytic gradient algorithm for the long-range-corrected (lrc-) XYG3 type of doubly hybrid functionals has been derived and implemented. The introduction of a long-range second-order perturbation as the correction requires the modification of the Z-vector equations and the construction of a unique total Lagrangian of the method. It has been observed that lrc-XYG3 offers a better description in dispersion-dominant systems compared to XYG3, while lrc-XYGJ-OS shows a better overall performance in reproducing intermolecular geometries.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Xiaoxiao Lu, Lulu Li, Xiaoren Zhang, Bina Fu, Xin Xu, Dong H. Zhang
Summary: A comparison of atomistic dynamics between microsolvated and unsolvated reactions can reveal the precise role of solvent molecules and provide insights into how solvation influences chemical reactions. In this study, a full-dimensional analytical potential energy surface was developed for the F-(H2O) + CH3I reaction, enabling efficient dynamics simulations at a quantitatively accurate level. The computed S(N)2 reactivity suppression ratio of the monosolvated F-(H2O) + CH3I reaction exhibits an inverted-V shape as a function of collision energy, indicating the combined dynamical effects of interaction time, steric hindrance, and collision-induced dehydration. Furthermore, analysis suggests that the steric effect of the F-(H2O) + CH3I reaction mainly arises from dragging the F- anion away from the central C atom, rather than shielding F- from C. This study highlights the potential for rigorously investigating the role of solvents in more complex reactions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Multidisciplinary Sciences
Xiaoxiao Lu, Chenyao Shang, Lulu Li, Rongjun Chen, Bina Fu, Xin Xu, Dong H. Zhang
Summary: The authors of this study highlight the significance of base-induced elimination and bimolecular nucleophilic substitution reactions in physical organic chemistry. They provide evidence that the competing factor of elimination, rather than steric hindrance, determines the low reactivity of nucleophilic substitution reactions. This finding provides new insights into the dynamical origin of intrinsic reactivity in gas-phase organic chemistry.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Bozhu Chen, Xin Xu
Summary: In this study, polymorph discrimination for three different molecular crystals was investigated using energy decomposition analysis. The XO-PBC(XYG3:PBE) method was found to accurately predict stability orderings and energy ranges, highlighting its potential application in polymorph control.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Zhenyu Zhu, Xin Xu
Summary: Static polarizability is crucial for describing optical phenomena and intermolecular interactions, as well as evaluating the accuracy of electronic structure methods. However, the current lack of polarizability data sets including diverse species and high-quality reference data is a challenge. In this study, we calibrated the reference data of two existing data sets (HR46 and T145) for molecules up to 15 atoms. By applying focal-point analysis, we achieved accurate isotropic and anisotropic polarizability calculations and obtained reference data close to CCSD(T)/aug-cc-pCV[Q5]Z quality. These reference data are valuable for future assessment and benchmark studies of electronic structure methods, particularly density functional approximations.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Yuqi Yang, Tonghao Shen, Xin Xu
Summary: First-principles-based micro-kinetic modeling is an important tool for designing heterogeneous catalysts. The combination of density functional theory (DFT) calculations and mean-field micro-kinetic modeling (MF-MKM) provides theoretical understandings and predictions, but sometimes yields undesired results. Understanding the success and failure of this approach is crucial for improving its accuracy.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Zheng Chen, Zhangyun Liu, Xin Xu
Summary: This study investigates the dynamic evolution of metal-support coordination in single atom catalysts and reveals that it can change the electronic structure of the active center, thereby enhancing or weakening the metal-adsorbate bonding. This effect has potential implications for increasing catalyst activity.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Yingrui Zhang, Ziwei Ye, Chunchun Li, Qinglu Chen, Wafaa Aljuhani, Yiming Huang, Xin Xu, Chunfei Wu, Steven E. J. Bell, Yikai Xu
Summary: This article introduces a method for the preparation of Pickering emulsions without the use of chemical modifiers. By using a combination of stabilizer particles and unmodified functional particles, Pickering emulsions can be constructed. This method not only unlocks the potential of Pickering emulsions, but also allows for a wide range of applications including plasmonic sensing and interfacial catalysis.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Medicinal
Jiaqi Liu, Jian Wan, Yanliang Ren, Xubo Shao, Xin Xu, Li Rao
Summary: This paper proposes a new method for predicting protein-ligand binding affinity called DOX_BDW, which takes into account the solvation effects and is particularly suitable for covalent binding situations and high-throughput screening scenarios in drug design. The performance of DOX_BDW is superior to current empirical scoring functions, with affordable computational cost and remarkable accuracy.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Review
Chemistry, Physical
Sai Duan, Xin Xu
Summary: Scanning tunneling microscope (STM) is an atomic-scale characterization tool that requires close cooperation between high-resolution measurements and accurate simulations. Recent progress in considering the effects of both tip and substrate in STM simulations provides an accurate analysis of measured high-resolution STM results and rational designs experimental protocols for complex chemical systems. This Perspective aims to stimulate broad interest in advanced STM simulations and highlight the way forward for STM investigations involving complex geometrical and electronic structures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Fengyu Li, Yuwei Zhang, Fei Xia, Xin Xu
Summary: The global spread of COVID-19 has had a severe impact on human health, resulting in numerous deaths. Using molecular dynamics (MD) simulations, researchers have developed an ultra-coarse-grained (UCG) model of the SARS-CoV-2 virion and a hybrid all-atom and UCG (AA/UCG) virion model to investigate the pathogenic mechanisms and protein interactions. The simulation results highlight the importance of developing multiscale models to study the functions of proteins in biomolecular complexes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Yuan Fang, Ren Hu, Jin-Yu Ye, Hang Qu, Zhi-You Zhou, Sai Duan, Zhong-Qun Tian, Xin Xu
Summary: The detailed structure of the water layer in the inner Helmholtz plane of a solid/aqueous solution interface is critical for understanding the electrochemical and catalytic performances of electrode materials. In this study, the interfacial water structure was investigated with the specific adsorption of p-nitrobenzoic acid on Au(111) surface. It was found that the protruding infrared band observed in the electrochemical infrared spectra is attributed to the surface-enhanced stretching mode of water molecules hydrogen-bonded to the adsorbed p-nitrobenzoate ions. The structure of the water layer is determined by both hydrogen-bonding interactions and coverages of specifically adsorbed p-nitrobenzoate.
Article
Chemistry, Physical
Zheng Chen, Zhangyun Liu, Xin Xu
Summary: The traditional trial-and-error approach is insufficient for catalyst development in energy and environmental challenges. Rational catalyst design, particularly using first-principles, has become important. Microkinetic modeling is necessary to correlate microscopic properties with macroscopic performance of catalysts, but current methods need improvement for accuracy and efficiency. The XPK method has been developed to accurately simulate complex heterogeneous catalytic processes. The formulation of free energy landscape (FEL) helps understand the impact of local surface coverages on macroscopic measures.
Article
Chemistry, Physical
Xue Yang, Zhangyun Liu, Boxu Gao, Zheng Chen, Kexin Yan, Sinong Wang, Yujian Xia, Yahong Zhang, Lei Wang, Xin Xu, Yi Tang
Summary: In this study, it was found that Co2+(Ba2+)-exchanged faujasite zeolites can efficiently catalyze the epoxidation of styrene with molecular oxygen. Through detailed experimental characterizations and calculations, the research team revealed the binuclear nature of the active sites, which is of great significance for optimizing oxidation catalysts.
Article
Chemistry, Multidisciplinary
Feifei Qiu, Zu-Yong Gong, Dongwei Cao, Ce Song, Guangjun Tian, Sai Duan, Yi Luo
Summary: Tip-enhanced fluorescence excitation (TEFE) is a new technique that utilizes highly confined plasmonic field to directly visualize the vibronic effect of a single molecule in real space for arbitrary excited states. Numerical simulations confirm that TEFE can identify vibronic couplings originating from Herzberg-Teller active modes.
