In this study, a verified process of the "grafting from" approach using surface initiated atom transfer radical polymerization was applied for the modification of a graphene oxide (GO) surface. This approach provides simultaneous grafting of poly(2-(trimethylsilyloxy)ethyl methacrylate) (PHEMATMS) chains and a controllable reduction of the GO surface. This allows the fine tuning of its electrical conductivity, which is a crucial parameter for applications of such hybrid composite particles in electrorheological (ER) suspensions. The successful coating was confirmed by transmission electron microscopy and Fourier-transform infrared spectroscopy. The molecular characteristics of PHEMATMS were characterized by gel permeation chromatography. ER performance was elucidated using a rotational rheometer under various electric field strengths and a dielectric spectroscopy to demonstrate the direct impact of both the relaxation time and dielectric relaxation strength on the ER effectivity. Enhanced compatibility between the silicone oil and polymer-modified GO particles was investigated using contact angle measurements and visual sedimentation stability determination. It was clearly proven that the modification of the GO surface improved the ER capability of the system due to the tunable conductivity during the surface-initiated atom transfer radical polymerization (SI-ATRP) process and the enhanced compatibility of the GO particles, modified by polymer containing silyl structures, with silicone oil. These unique ER properties of this system appear very promising for future applications in the design of ER suspensions.
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http://dx.doi.org/10.3390/nano9020308 | DOI Listing |
J Am Chem Soc
January 2025
Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States.
Terminal metal-phosphorus (M-P) complexes are of significant contemporary interest as potential platforms for P-atom transfer (PAT) chemistry. Decarbonylation of metal-phosphaethynolate (M-PCO) complexes has emerged as a general synthetic approach to terminal M-P complexes. M-P complexes that are stabilized by strong M-P multiple bonds are kinetically persistent and isolable.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, USA.
Identifying informative low-dimensional features that characterize dynamics in molecular simulations remains a challenge, often requiring extensive manual tuning and system-specific knowledge. Here, we introduce geom2vec, in which pretrained graph neural networks (GNNs) are used as universal geometric featurizers. By pretraining equivariant GNNs on a large dataset of molecular conformations with a self-supervised denoising objective, we obtain transferable structural representations that are useful for learning conformational dynamics without further fine-tuning.
View Article and Find Full Text PDFDalton Trans
January 2025
Beijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, P. R. China.
Nowadays, benzimidazole and its derivatives are widely assembled into multifunctional materials with various properties such as mechanochromism, photochromism, thermochromism and electrochromism. Herein, two novel zinc(II) coordination compounds, [Zn(L)Br]·2HO (1) and [Zn(L)Cl]·2HO (2) (L = tetra(1-benzo[]imidazol-2-yl)ethene), have been constructed one-pot facile synthesis from bis(1-benzo[]imidazol-2-yl)methane (L) and zinc(II) salts. The ligand L with a CC double bond was formed by C-C coupling of two sp-C atoms of L in solvothermal synthesis, which provides a new strategy to generate the conjugation system conveniently.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
The University of Oklahoma, Chemistry and Biochemistry, 101 Stephenson Parkway, 73019, Norman, UNITED STATES OF AMERICA.
Phototherapy - which includes photothermal therapy (PTT) and photodynamic therapy (PDT) - has evoked interest as a promising cancer treatment modality on account of its noninvasiveness, spatiotemporal precision, and minimal side effects. C. Wang et al.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1, 8093 Zürich, Switzerland.
Organic redox systems that can undergo oxidative and reductive (ambipolar) electron transfer are elusive yet attractive for applications across synthetic chemistry and energy science. Specifically, the use of ambipolar redox systems in proton-coupled electron transfer (PCET) reactions is largely unexplored but could enable "switchable" reactivity wherein the uptake and release of hydrogen atoms are controlled using a redox stimulus. Here, we describe the synthesis and characterization of an ambipolar functionalized terthiophene (TTH) bearing methyl thioether and phosphine oxide groups that exhibits switchable PCET reactivity.
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