Fluid Phase Equilibria, Journal Year: 2023, Volume and Issue: 575, P. 113931 - 113931
Published: Aug. 20, 2023
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)
Published: March 13, 2024
The quantification of Lewis acidity is fundamental and applied importance in chemistry. However, if neutral charged acids are compared, a coherent ranking has been elusive, severe uncertainties were accepted. With this study, we present systematic computational analysis base affinities 784 mono-, di- tricationic their comparison with 149 representative acids. Evaluating vacuum fluoride ion (FIA) reveals charge-caused clustering that prohibits any meaningful ranking. Instead, solvation-corrected FIA
Language: Английский
Citations
11
Fluid Phase Equilibria, Journal Year: 2024, Volume and Issue: unknown, P. 114250 - 114250
Published: Oct. 1, 2024
Language: Английский
Citations
6
The Journal of Physical Chemistry A, Journal Year: 2024, Volume and Issue: 128(31), P. 6440 - 6449
Published: July 25, 2024
A new hybrid discrete-continuum approach named the cluster-continuum static approximation (CCSA) has been proposed for acetonitrile solvent. The continuum part uses conductor-like polarizable model electrostatic and a surface area-dependent term nonelectrostatic solvation. CCSA includes only one explicit solvent molecule damping function, which makes method reduce to pure solvation in case of weaker potential mean force solute-solvent interaction. performance was tested 22 anions cations, including challenge species that cannot be adequately described by comparison done with widely used density (SMD) model. For anions, reduces same as SMD model, standard deviation signed error (SD-MSE) 2.7 kcal mol
Language: Английский
Citations
5
The Journal of Physical Chemistry A, Journal Year: 2023, Volume and Issue: 127(48), P. 10268 - 10281
Published: Nov. 27, 2023
Although charged solutes are common in many chemical systems, traditional solvation models perform poorly calculating energies of ions. One major obstacle is the scarcity experimental data for solvated In this study, we release an experiment-based aqueous ionic energy set, IonSolv-Aq, that contains hydration free 118 anions and 155 cations, more than 2 times larger set singly ions contained 2012 Minnesota Solvation Database commonly used benchmarking studies. We discuss sources systematic uncertainty use to examine accuracy popular implicit COSMO-RS SMD predicting water. Our results indicate most modeling errors correctable with empirical parameters. two offsets: one across all depends on functional group ionization site. After correcting these offsets, predicted using 3.1 kcal mol-1 MAE against a challenging test 1.7 (about 3% relative error) filtered set. The performance similar, those same sets 2.7 mol-1. These underscore importance compiling improve model parametrization fairly assess performance.
Language: Английский
Citations
10
Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(22)
Published: March 13, 2024
Abstract The quantification of Lewis acidity is fundamental and applied importance in chemistry. However, if neutral charged acids are compared, a coherent ranking has been elusive, severe uncertainties were accepted. With this study, we present systematic computational analysis base affinities 784 mono‐, di‐ tricationic their comparison with 149 representative acids. Evaluating vacuum fluoride ion (FIA) reveals charge‐caused clustering that prohibits any meaningful ranking. Instead, solvation‐corrected FIA solv identified as metric overcomes charge sensitivity balanced manner, allowing for evaluation across varying states. Analyzing the impact molecular volume on solvation‐induced damping provides rationales trends guidelines choice or design cationic condensed phase. Exploring alternative scales, explicit counteranion effects, selected experimental case studies reaffirms advantages most versatile practical approach quantitative general (thermodynamic) acidity.
Language: Английский
Citations
0
Industrial & Engineering Chemistry Research, Journal Year: 2024, Volume and Issue: 63(17), P. 7727 - 7742
Published: April 17, 2024
Charged microgels are promising for different applications due to their multiresponsive nature. Achieving tailored microgel properties necessitates synthesis monitoring and computational modeling. However, process analytics of multicomponent solutions occurring during charged face challenges. Furthermore, existing modeling approaches employ steady-state models while lacking fully determined kinetic parameter values. In this contribution, we use Raman spectroscopy indirect hard measure concentrations samples obtained the predict monomer content. Additionally, derive a dynamic model including pH dependence. Based on data from spectroscopy, calorimetry, quantum mechanical computations, estimate complete set reaction values poly(N-isopropylacrylamide-co-methacrylic) acid microgels. The allows simulation synthesis, revealing effects changes. Thus, work represents an important step toward model-based production
Language: Английский
Citations
0
Fluid Phase Equilibria, Journal Year: 2023, Volume and Issue: 575, P. 113931 - 113931
Published: Aug. 20, 2023
Language: Английский
Citations
0