We report on the structure of dendritic polyelectrolytes accompanied by counterions in a good, salt-free, implicit solvent using Langevin dynamics simulations and a Flory-type approach. Our focus is on the modification of charged dendrimer conformations via the strength of electrostatic interactions and the counterion excluded volume. We study the effects caused by charges by varying the reduced Bjerrum length, λ, between the extremes of weak and strong electrostatic interactions. The counterion excluded volume was controlled by the size of ions. We investigate counterions ranging from conventional ones, with the size comparable to the monomer size, to bulky ions. Our results indicate that, as compared to neutral dendrimers, dendritic polyelectrolytes exist in swollen conformations, and the degree of swelling changes non-monotonically with increasing λ. For weak electrostatic couplings, counterion density within dendrimers is minor and their radius of gyration subtly exceeds the size of neutral dendrimers. For intermediate electrostatic couplings, Coulomb attraction between opposite charges promotes absorption of ions into dendrimers' pervaded volume and counterion condensation on charged monomers. As a result, counterion density inside dendrimers abruptly increases and the ionic size starts to play a crucial role. In this regime, we observe that swelling of dendrimers reaches its maximum and is more pronounced for bulky counterions. For strong electrostatic couplings, complete condensation of conventional counterions proceeds, whereas for bulky ions condensation remains partial. In this regime, dendrimers deswell. In particular, in the presence of conventional ions, dendrimers collapse into globules, while, for bulky counterions, deswelling is suppressed.
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January 2025
MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
The photocatalytic activity of lead-free perovskite heterostructures currently suffers from low efficiency due to the lack of active sites and the inadequate photogenerated carrier separation, the latter of which is hindered by slow charge transfer at the heterostructure interfaces. Herein, a facile strategy is reported for the construction of lead-free halide-perovskite-based heterostructure with swift interfacial charge transfer, achieved through direct partial conversion of 2D antimony oxybromide SbOBr to generate CsSbBr/SbOBr heterostructure. Compared to the traditional electrostatic self-assembly method, this approach endows the CsSbBr/SbOBr heterostructure with a tightly interconnected interface through in situ partial conversion, significantly accelerating interfacial charge transfer and thereby enhancing the separation efficiency of photogenerated carriers.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Departament de Farmàcia i Tecnologia Farmacèutica, i Fisicoquímica, Facultat de Farmàcia i Ciències de l'Alimentació, Universitat de Barcelona (UB), 08028 Barcelona, Spain.
Incorporation of environment and vibronic effects in simulations of optical spectra and excited state dynamics is commonly done by combining molecular dynamics with excited state calculations, which allows to estimate the spectral density describing the frequency-dependent system-bath coupling strength. The need for efficient sampling, however, usually leads to the adoption of classical force fields despite well-known inaccuracies due to the mismatch with the excited state method. Here, we present a multiscale strategy that overcomes this limitation by combining EMLE simulations based on electrostatically embedded ML potentials with the QM/MMPol polarizable embedding model to compute the excited states and spectral density of 3-methyl-indole, the chromophoric moiety of tryptophan that mediates a variety of important biological functions, in the gas phase, in water solution, and in the human serum albumin protein.
View Article and Find Full Text PDFACS Nano
January 2025
College of Animal Science and Technology, Northeast Agricultural University, Harbin 150030, P. R. China.
The emergence of multidrug-resistant (MDR) pathogens, coupled with the limited effectiveness of existing antibiotics in eradicating biofilms, presents a significant threat to global health care. This critical situation underscores the urgent need for the discovery and development of antimicrobial agents. Recently, peptide-derived antimicrobial nanomaterials have shown promise in combating such infections.
View Article and Find Full Text PDFInt J Biol Macromol
January 2025
Department of Environmental Engineering, Kyungpook National University, 80 Daehak-ro, Buk-gu, Daegu 41566, Republic of Korea. Electronic address:
This study describes the preparation of novel hybrid aerogels derived from gelatin (Gel), incorporating Br-functionalized zirconium-based metal-organic framework (UiO-66-Br; MOF) as modifying agent to effectively eliminate phosphate and fluoride ions from aqueous environments. The adsorption performance of MOF decorated Gel (Gel-xMOF) hybrid aerogels was investigated under different conditions, including agitation time, adsorbent dosage, solution pH, initial phosphate and fluoride concentrations, coexisting ions, and temperature. The functional groups of the gelatin network, coupled with UiO-66-Br, enhanced the adsorption performance of phosphate and fluoride ions from aqueous solutions.
View Article and Find Full Text PDFSmall
January 2025
Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, P. R. China.
Although Silicon monoxide (SiO) is regarded as the most promising next-generation anode material, the large volume expansion, poor conductivity, and low initial Coulombic efficiency (ICE) severely hamper its commercialization application. Designing a multilayer conductive skeleton combined with advanced prelithiation technology is considered an effective approach to address these problems. Herein, a reliable strategy is proposed that utilizes MXene and carbon nanotube (CNT) as dual-conductive skeletons to encapsulate SiO through simple electrostatic interaction for high-performance anodes in LIBs, while also performing chemical prelithiation.
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