In addition to modifying surface properties, self-assembled monolayers, SAMs, on nanoparticles can selectively incorporate small molecules from the surrounding solution. This selectivity has been used in the design of substrate-specific catalytic systems but its degree has not been quantified. This work uses catalytic centers embedded in on-nanoparticle hydrophobic SAMs to monitor and quantify the partitioning of molecules between the bulk solvent and these monolayers. A combination of experiments and theory allows us to relate the logarithm of the incorporation-into-SAM constant to the "bulk" log values, characterizing the incoming substrates. These results are in line with classic, semi-empirical linear free energy relationships between partitioning solvent systems; in this way, they substantiate the view of nanoscopic on-particle SAMs acting akin to a bulk solvent phase.
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http://dx.doi.org/10.1039/d2nr06341g | DOI Listing |
J Phys Chem A
January 2025
Department of Chemistry and Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States.
Theoretical simulations of electron detachment processes are vital for understanding chemical redox reactions, semiconductor and electrochemical properties, and high-energy radiation damage. However, accurate calculations of ionized electronic states are very challenging due to their open-shell nature, importance of electron correlation effects, and strong interactions with chemical environment. In this work, we present an efficient approach based on algebraic diagrammatic construction theory with polarizable embedding that allows to accurately simulate ionized electronic states in condensed-phase or biochemical environments (PE-IP-ADC).
View Article and Find Full Text PDFJ Phys Chem B
January 2025
Department of Chemistry, Kansas State University, Manhattan, Kansas 66506, United States.
Ion atmospheres play a critical role in modulating the interactions between charged components in solutions. However, a detailed description of the nature of ion atmospheres remains elusive. Here, we use Kirkwood-Buff theory, an exact theory of solution mixtures, together with a series of local and bulk electroneutrality constraints to provide relationships between all the net ion-ion distributions in bulk electrolyte mixtures.
View Article and Find Full Text PDFEuroasian J Hepatogastroenterol
December 2024
Department of Gastroenterology and Metabology, Ehime University Graduate School of Medicine, Ehime, Japan.
Objectives: To predict and characterize the three-dimensional (3D) structure of protein arginine methyltransferase 2 (PRMT2) using homology modeling, besides, the identification of potent inhibitors for enhanced comprehension of the biological function of this protein arginine methyltransferase (PRMT) family protein in carcinogenesis.
Materials And Methods: An method was employed to predict and characterize the three-dimensional structure. The bulk of PRMTs in the PDB shares just a structurally conserved catalytic core domain.
ACS Nano
January 2025
Ministry of Industry and Information Technology Key Lab of Micro-Nano Optoelectronic Information System, Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems, Harbin Institute of Technology (Shenzhen), Shenzhen, Guangdong 518055, China.
The power conversion efficiencies (PCEs) of polycrystalline perovskite solar cells (PC-PSCs) have now reached a plateau after a decade of rapid development, leaving a distinct gap from their Shockley-Queisser limit. To continuously mitigate the PCE deficit, nonradiative carrier losses resulting from defects should be further optimized. Single-crystal perovskites are considered an ideal platform to study the efficiency limit of perovskite solar cells due to their intrinsically low defect density, as demonstrated in bulk single crystals.
View Article and Find Full Text PDFAcc Chem Res
January 2025
Center for Molecular Spectroscopy and Dynamics, Institute for Basic Science, Seoul 02841, Korea.
ConspectusWater-in-salt electrolytes (WiSEs) are promising electrolytes for next-generation lithium-ion batteries (LIBs), offering critical advantages like nonflammability and improved safety. These electrolytes have extremely high salt concentrations and exhibit unique solvation structures and transport mechanisms dominated by the formation of ion networks and aggregates. These ion networks are central to the performance of WiSEs, govern the transport properties and stability of the electrolyte, deviating from conventional dilute aqueous or organic electrolytes.
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