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ACS Medicinal Chemistry Letters Jun 2024Bfl-1 is overexpressed in both hematological and solid tumors; therefore, inhibitors of Bfl-1 are highly desirable. A DNA-encoded chemical library (DEL) screen against...
Bfl-1 is overexpressed in both hematological and solid tumors; therefore, inhibitors of Bfl-1 are highly desirable. A DNA-encoded chemical library (DEL) screen against Bfl-1 identified the first known reversible covalent small-molecule ligand for Bfl-1. The binding was validated through biophysical and biochemical techniques, which confirmed the reversible covalent mechanism of action and pointed to binding through Cys55. This represented the first identification of a cyano-acrylamide reversible covalent compound from a DEL screen and highlights further opportunities for covalent drug discovery through DEL screening. A 10-fold improvement in potency was achieved through a systematic SAR exploration of the hit. The more potent analogue compound was successfully cocrystallized in Bfl-1, revealing the binding mode and providing further evidence of a covalent interaction with Cys55.
PubMed: 38894895
DOI: 10.1021/acsmedchemlett.4c00113 -
Sensors (Basel, Switzerland) May 2024Acrylamide (AA), an odorless and colorless organic small-molecule compound found generally in thermally processed foods, possesses potential carcinogenic, neurotoxic,... (Review)
Review
Acrylamide (AA), an odorless and colorless organic small-molecule compound found generally in thermally processed foods, possesses potential carcinogenic, neurotoxic, reproductive, and developmental toxicity. Compared with conventional methods for AA detection, bio/chemical sensors have attracted much interest in recent years owing to their reliability, sensitivity, selectivity, convenience, and low cost. This paper provides a comprehensive review of bio/chemical sensors utilized for the detection of AA over the past decade. Specifically, the content is concluded and systematically organized from the perspective of the sensing mechanism, state of selectivity, linear range, detection limits, and robustness. Subsequently, an analysis of the strengths and limitations of diverse analytical technologies ensues, contributing to a thorough discussion about the potential developments in point-of-care (POC) for AA detection in thermally processed foods at the conclusion of this review.
Topics: Acrylamide; Biosensing Techniques; Point-of-Care Systems; Humans; Food Analysis; Food Contamination
PubMed: 38894291
DOI: 10.3390/s24113501 -
Research Progress of Molecular Simulation in Acrylamide Polymers with High Degree of Polymerization.Molecules (Basel, Switzerland) May 2024Acrylamide polymers with a high degree of polymerization are widely used in petroleum production. It is of great significance to study the oil displacement mechanism of... (Review)
Review
Acrylamide polymers with a high degree of polymerization are widely used in petroleum production. It is of great significance to study the oil displacement mechanism of acrylamide polymers with a high degree of polymerization from the micro level. In recent years, the rapid development of computer molecular simulation technology has filed the gaps in macroscopic experiments and theories. This technology has been highly valued in the study of the molecular behaviour of polymer systems. In this paper, the research progress of molecular simulation applied to high-polymerization-degree acrylamide polymer is summarized. The application status of acrylamide polymer flooding, the analysis of polymer flooding mechanisms, and the research progress of molecular simulation in acrylamide linear and crosslinked polymers are expounded. Finally, the development prospect of acrylamide polymer research is given, and suggestions are put forward in terms of simulation direction and simulation tools.
PubMed: 38893464
DOI: 10.3390/molecules29112589 -
Polymers May 2024A series of stimuli-responsive fluorescent hydrogels were successfully synthesized via micelle radical copolymerization of hydrophilic acrylamide (AM), hydrophobic...
A series of stimuli-responsive fluorescent hydrogels were successfully synthesized via micelle radical copolymerization of hydrophilic acrylamide (AM), hydrophobic chromophore terpyridine-based monomer (TPY), and -isopropylacrylamide (NIPAM). These hydrogels presented blue emissions (423-440 nm) under room temperature, which is caused by the π-π* transition of the conjugated structures. Once the ambient temperature was increased to 55 °C, the fluorescence color changed from blue (430 nm) to pink (575 nm) within 10 min, subsequently to yellow (535 nm), and eventually back to pink. The thermal-responsive properties are attributed to the transition of the TPY units from unimer to dimer aggregation via the intermolecular charge transfer complex at high temperatures. The hydrogels showed pH-responsive properties. The emission peak of the hydrogel exhibited a blue shift of ~54 nm from neuter conditions to acidic conditions, while a 6 nm red shift to an alkaline environment was observed. The hydrogels demonstrated an obvious change in fluorescence intensity and wavelength upon adding different metal ions, which is caused by the coordination between the terpyridine units incorporated on the backbones and the metal ions. As a consequence, the hydrogels presented a sharp quenching fluorescence interaction with Fe, Fe, Cu, Hg, Ni, and Co, while it exhibited an enhanced fluorescence intensity interaction with Sn, Cd, and Zn. The microstructural, mechanical, and rheological properties of these luminescent hydrogels have been systematically investigated.
PubMed: 38891465
DOI: 10.3390/polym16111519 -
Polymers May 2024Polymer gels are cross-linked polymer networks swollen by a solvent. These cross-linked networks are interconnected to produce a three-dimensional molecular framework....
Polymer gels are cross-linked polymer networks swollen by a solvent. These cross-linked networks are interconnected to produce a three-dimensional molecular framework. It is this cross-linked network that provides solidity to the gel and helps to hold the solvent in place. The present work deals with the fabrication of polybenzoxazine carbon (PBzC)-based gels that could function as a solid electrode in flexible supercapacitors (SCs). With the advantage of molecular design flexibility, polybenzoxazine-based carbon containing different hetero-atoms was synthesized. A preliminary analysis of PBzC including XRD, Raman, XPS, and SEM confirmed the presence of hetero-atoms with varying pore structures. These PBz-carbons, upon reaction with polyvinyl alcohol (PVA) and acrylamide (AAm), produced a composite polymer hydrogel, PVA/poly (AAm)/PBzC. The performance of the synthesized hydrogel was analyzed using a three-electrode system. PVA/poly (AAm)/PBzC represented the working electrode. The inclusion of PBzC within the PVA/poly (AAm) matrix was evaluated by cyclic voltammetry and galvanostatic charge/discharge measurements. A substantial increase in the CV area and a longer charge/discharge time signified the importance of PBzC inclusion. The PVA/poly (AAm)/PBzC electrode exhibited larger specific capacitance (C) of 210 F g at a current density of 0.5 A g when compared with the PVA/poly (AAm) electrode [Cs = 92 F g]. These improvements suggest that the synthesized composite hydrogel can be used in flexible supercapacitors requiring light weight and wearability.
PubMed: 38891410
DOI: 10.3390/polym16111463 -
Foods (Basel, Switzerland) May 2024In this study, a critical review was carried out using the Web of Science Core Collection database to analyse the scientific literature published to date to identify... (Review)
Review
In this study, a critical review was carried out using the Web of Science Core Collection database to analyse the scientific literature published to date to identify lines of research and future perspectives on the presence of chemical pollutants in beer brewing. Beer is one of the world's most popular drinks and the most consumed alcoholic beverage. However, a widespread challenge with potential implications for human and animal health is the presence of physical, chemical, and/or microbiological contaminants in beer. Biogenic amines, heavy metals, mycotoxins, nitrosamines, pesticides, acrylamide, phthalates, bisphenols, microplastics, and, to a lesser extent, hydrocarbons (aliphatic chlorinated and polycyclic aromatic), carbonyls, furan-derivatives, polychlorinated biphenyls, and trihalomethanes are the main chemical pollutants found during the beer brewing process. Pollution sources include raw materials, technological process steps, the brewery environment, and packaging materials. Different chemical pollutants have been found during the beer brewing process, from barley to beer. Brewing steps such as steeping, kilning, mashing, boiling, fermentation, and clarification are critical in reducing the levels of many of these pollutants. As a result, their residual levels are usually below the maximum levels allowed by international regulations. Therefore, this work was aimed at assessing how chemical pollutants appear and evolve in the brewing process, according to research developed in the last few decades.
PubMed: 38890939
DOI: 10.3390/foods13111709 -
Journal of Controlled Release :... Jul 2024
Corrigendum to "Peptide conjugation enhances the cellular co-localization, but not endosomal escape, of modular poly (acrylamide-co-methacrylic acid) nanogels" [Journal of Controlled Release, 329, 1162-1171].
PubMed: 38890014
DOI: 10.1016/j.jconrel.2024.06.032 -
ACS Applied Materials & Interfaces Jun 2024Bilayer hydrogels, endowed with multiresponsive and switchable color-changing properties, have garnered significant attention for bioinspired artificial intelligent...
Bilayer hydrogels, endowed with multiresponsive and switchable color-changing properties, have garnered significant attention for bioinspired artificial intelligent materials. However, the design and fabrication of such hydrogels that can fully mimic the adaptation of the live organism, ., simultaneous changes in shape, fluorescent, and/or visible color, still remain significant challenges. Herein, a multiresponsive (e.g., temperature, salt, and pH) and multiadaptive (shape, fluorescent color, and visible color changes) hydrogel was fabricated by employing monomers featuring pH-responsive fluorescence 4-(2-(4-(dimethylamino) phenyl)-1-isocyanovinyl) phenol (DP) and switchable color-changing 4-(2-sulfethyl) -1-(4-vinylbenzyl) pyridinium betaine (VPES). The bilayer hydrogel comprises a temperature- and pH-responsive gel layer, poly(-isopropylacrylamide--2-(dimethylamino) ethyl methacrylate), along with a pH-, temperature-, and salt-responsive gel layer, poly(acrylamide--2-(dimethylam2ino)ethyl methacrylate--VPES)@DP. Due to the opposite swelling/shrinking behavior between the two layers, the prepared hydrogel exhibits shape changes in response to thermal, salt, and pH stimuli, along with switchable fluorescent color and visible color change that originate from DP and polyVPES, respectively. Apart from multiresponsive behavior, this hydrogel also shows an excellent antifatigue property and high sensitivity, which makes it hold significant potential in many applications. We anticipate that this strategy to realize multiresponsive capability in this work can also inspire the design of the biomimetic smart materials.
PubMed: 38888298
DOI: 10.1021/acsami.4c06121 -
Journal of Chemical Information and... Jun 2024Molecularly imprinted polymers (MIPs) have emerged as bespoke materials with versatile molecular applications. In this study, we propose a proof of concept for a...
Molecularly imprinted polymers (MIPs) have emerged as bespoke materials with versatile molecular applications. In this study, we propose a proof of concept for a methodology employing molecular dynamics (MD) simulations to guide the selection of functional monomers for curcuminoid binding in MIPs. Curcumin, demethoxycurcumin, and bisdemethoxycurcumin are phenolic compounds widely employed as spices, pigments, additives, and therapeutic agents, representing the three main curcuminoids of interest. Through MD simulations, we investigated prepolymerization mixtures composed of various functional monomers, including acrylamide (ACA), acrylic acid (AA), methacrylic acid (MAA), and -vinylpyrrolidone (NVP), with ethylene glycol dimethacrylate (EGDMA) as the cross-linker and acetonitrile as the solvent. Curcumin was selected as the template molecule due to its structural similarity to the other curcuminoids. Notably, the prepolymerization mixture containing NVP as the functional monomer demonstrated superior molecular recognition capabilities toward curcumin. This observation was supported by higher functional monomer molecules surrounding the template, a lower total nonbonded energy between the template and monomer, and a greater number of hydrogen bonds in the aggregate. These findings suggest a stronger affinity between the functional monomer NVP and the template. We synthesized, characterized, and conducted binding tests on the MIPs to validate the MD simulation results. The experimental binding tests confirmed that the MIP-NVP exhibited higher binding capacity. Consequently, based on MD simulations, our computational methodology effectively guided the selection of the functional monomer, leading to MIPs with binding capacity for curcuminoids. The outcomes of this study provide a valuable reference for the rational design of MIPs through MD simulations, facilitating the selection of components for MIPs. This computational approach holds the potential for extension to other templates, establishing a robust methodology for the rational design of MIPs.
PubMed: 38888100
DOI: 10.1021/acs.jcim.4c00775 -
Angewandte Chemie (International Ed. in... Jun 2024The radical Truce-Smiles rearrangement is a straightforward strategy for incorporating aryl groups into organic molecules for which asymmetric processes remains rare. By...
The radical Truce-Smiles rearrangement is a straightforward strategy for incorporating aryl groups into organic molecules for which asymmetric processes remains rare. By employing a readily available and non-expensive chiral auxiliary, we developed a highly efficient asymmetric photocatalytic acyl and alkyl radical Truce-Smiles rearrangement of α-substituted acrylamides using tetrabutylammonium decatungstate (TBADT) as a hydrogen atom-transfer photocatalyst, along with aldehydes or C-H containing precursors. The rearranged products exhibited excellent diastereoselectivities (7:1 to >98:2 d.r.) and chiral auxiliary was easily removed. Mechanistic studies allowed understanding the transformation in which density functional theory (DFT) calculations provided insights into the stereochemistry-determining step.
PubMed: 38887967
DOI: 10.1002/anie.202408154