Development of Accurate Force Fields for Mg and Triphosphate Interactions in ATP·Mg and GTP·Mg Complexes.

In cells, adenosine triphosphate (ATP) and guanosine triphosphate (GTP) molecules typically form tricoordinated or bicoordinated ATP·Mg or GTP·Mg complexes with Mg ions and bind to proteins, participating in and regulating many important cellular functions. The accuracy of their force field parameters plays a crucial role in studying the function-related conformations of ATP·Mg or GTP·Mg using molecular dynamics (MD) simulations. The parameters developed based on the methyl triphosphate model in existing AMBER force fields cannot accurately describe the conformational distribution of tricoordinated or bicoordinated ATP·Mg or GTP·Mg complexes in solution.

A practical approach to quantitative analytical surface-enhanced Raman spectroscopy.

Many of the features of SERS, such as its high sensitivity, molecular specificity and speed of analysis make it attractive as an analytical technique. However, SERS currently remains a specialist technique which has not yet entered the mainstream of analytical chemistry. Therefore, this review draws out the underlying principles for analytical SERS and provides practical tips and tricks for SERS quantitation.

Photocatalytic low-temperature defluorination of PFASs.

Polyfluoroalkyl and perfluoroalkyl substances (PFASs) are found in many everyday consumer products, often because of their high thermal and chemical stabilities, as well as their hydrophobic and oleophobic properties. However, the inert carbon-fluorine (C-F) bonds that give PFASs their properties also provide resistance to decomposition through defluorination, leading to long-term persistence in the environment, as well as in the human body, raising substantial safety and health concerns. Despite recent advances in non-incineration approaches for the destruction of functionalized PFASs, processes for the recycling of perfluorocarbons (PFCs) as well as polymeric PFASs such as polytetrafluoroethylene (PTFE) are limited to methods that use either elevated temperatures or strong reducing reagents.

Challenges with Literature-Derived Data in Machine Learning for Yield Prediction: A Case Study on Pd-Catalyzed Carbonylation Reactions.

The application of machine learning (ML) to predict reaction yields has shown remarkable accuracy when based on high-throughput computational and experimental data. However, the accuracy significantly diminishes when leveraging literature-derived data, highlighting a gap in the predictive capability of the current ML models. This study, focusing on Pd-catalyzed carbonylation reactions, reveals that even with a data set of 2512 reactions, the best-performing model reaches only an of 0.

Sacrificing Surfactants to Improve Oil Recovery: A Fluid Density Functional Theory Study.

In the chemically enhanced oil recovery (CEOR) processes, heavy components in crude oil, such as asphaltenes, adhere to reservoir rocks, significantly impeding crude oil extraction. Surfactants are frequently utilized to improve oil recovery due to their ability to reduce interfacial tension (IFT) and modify surface wettability. Nevertheless, indiscriminate surfactant usage may result in resource wastage and hinder the attainment of optimal recovery outcomes.

Allylation of Lactol in Water.

We developed a water-promoted cross-coupling of 3-hydroxyisobenzofuran-1(3)-ones and allylic boronates under biocompatible conditions. This approach facilitates the synthesis of diverse 3-allylic phthalides with high yields and exceptional selectivity in a metal-free manner. The versatility and practicality of this protocol underscore its significant potential for drug development and applications in medicinal chemistry.

Single-Electrode Flow Cell for Electrochemiluminescent Flow Analysis.

Flow injection analysis and liquid chromatography are frequently combined with electrochemiluminescence (ECL) for flow analysis. Almost all electrochemistry flow analyses employ traditional three-electrode electrochemical flow cells which have working electrode, counter electrode, and reference electrode; however, it is expensive and difficult to fabricate a traditional three-electrode electrochemical flow cell and inconvenient to renew the electrode. In this study, we have developed a single-electrode flow cell using commercially available conductive polyethylene film as the only electrode through potential differences induced by the electrode resistance for the first time.

Facile Alkyne Assembly-Enabled Functional Au Nanosheets for Photoacoustic Imaging-Guided Photothermal/Gene Therapy of Orthotopic Glioblastoma.

Treatment of glioblastoma (GBM) remains challenging due to the presence of blood-brain barrier (BBB) and tumor heterogeneity. Herein, Au nanosheets (AuNSs) functionalized with RGD peptides and small interfering RNA (siRNA), referred to as AuNSs-RGD-C≡C-siRNA (ARCR), are prepared to achieve multimodal therapy for GBM. The AuNSs with a large modifiable surface area, intriguing photothermal conversion efficiency (50.

Deamidation analysis of therapeutic drugs using matrix-assisted laser desorption ionization mass spectrometry and a novel algorithm QuanDA.

A robust deamidation quantification method, called QuanDA, was developed to quantify the spontaneous nonenzymatic deamidation of peptides based on the isotopic distribution change of peptides in matrix-assisted laser desorption ionization (MALDI) mass spectra and non-negative least squares calculation. The predictive model of QuanDA using theoretical spectra of pure un-deamidated and deamidated peptides for a series of simulated partial deamidated peptides is satisfying, with a coefficient of determination () and root mean squared error (RMSE) of 0.9914 and 0.

Selenenylsulfide covalent-directed chemistry for the detection of sulfhydryl groups using a diselenide fluorescent probe.

We report the development of a diglycosyldiselenide-based fluorescent probe for the rapid detection of sulfhydryl-containing biomolecules. The probe facilitates a chemoselective coupling reaction with sulfhydryl groups in aqueous buffer under ambient conditions, resulting in the formation of homogeneous Se-S conjugates within one hour. Using glutathione, a sulfhydryl-containing biomolecule, as a proof of concept, the probe achieved a detection limit of 0.

Rational Design of Advanced Gene Delivery Carriers: Macrophage Phenotype Matters.

Nucleic acid delivery in hard-to-transfect macrophages have attracted increasing attention in diverse applications such as defence against bacterial infection. Regulated by microenvironments in specific applications, macrophages have a heterogenous nature and exist in different phenotypes with diverse functions, e.g.

Dual Near-Infrared-Response S-Scheme Heterojunction with Asymmetric Adsorption Sites for Enhanced Nitrogen Photoreduction.

Photocatalytic nitrogen reduction reaction (PNRR) holds immense promise for sustainable ammonia (NH) synthesis. However, few photocatalysts can utilize NIR light that carries over 50% of the solar energy for NH production with high performance. Herein, a dual NIR-responsive S-scheme ZnCoS/FeS heterojunction photocatalyst is designed with asymmetric adsorption sites and excellent PNRR performance.

Modular Design and Scaffold-Synthesis of Multi-Functional Fluorophores for Targeted Cellular Imaging and Pyroptosis.

Fluorophores are essential tools for optical imaging and biomedical research. Their synthetic modification to incorporate new functions, however, remains a challenging task. Conventional strategies rely on linear synthesis in which a parent framework is gradually extended.

Gram-scale green synthesis of a highly stable cationic covalent organic framework for efficient and selective removal of ReO /TcO.

Covalent organic frameworks (COFs) have developed as efficient and selective adsorbents to mitigate TcO contamination. However, the eco-friendly and scalable production of COF-based adsorbents for the removal of TcO has not yet been reported. This study explores the potential of a cationic COF (TpDB-COF) synthesized a green hydrothermal method, achieving gram-scale yields per batch, thereby addressing a significant limitation of existing COF production methods.

HO-activated mitochondria-targeting photosensitizer for fluorescence imaging-guided combination photodynamic and radiotherapy.

Radiotherapy is a primary modality in cancer treatment but is accompanied by severe side effects to healthy tissues and radiation resistance to some extent. To overcome these limitations, we developed a HO-responsive photosensitizer, CyBT, which could be activated by the upregulated HO induced by radiotherapy, enabling near-infrared fluorescence imaging-guided combination photodynamic and radiotherapy. The synthesis of CyBT began with the covalent linkage of hemicyanine and a free radical TEMPO through the click reaction, which demonstrated superior photodynamic properties.

Tumor-specific delivery of clickable inhibitor for PD-L1 degradation and mitigating resistance of radioimmunotherapy.

Achieving selective and durable inhibition of programmed death ligand 1 (PD-L1) in tumors for T cell activation remains a major challenge in immune checkpoint blockade therapy. We herein presented a set of clickable inhibitors for spatially confined PD-L1 degradation and radioimmunotherapy of cancer. Using metabolic glycan engineering click bioorthogonal chemistry, PD-L1 expressed on tumor cell membranes was labeled with highly active azide groups.

Discovery of Chalcone Derivatives as Bifunctional Molecules with Anti-SARS-CoV-2 and Anti-inflammatory Activities.

Danshensu extracted with traditional Chinese medicine has a wide range of bioactivities. Danshensu containing a catechol moiety has a moderate inhibitory effect on SARS-CoV-2 3CL (IC = 2.2 μM) by a reversible covalent interaction and exhibits good anti-inflammatory activity.

Production of Branched Alkanes by Upcycling of Waste Polyethylene over Controlled Acid Sites of SO/ZrO-AlO Catalyst.

Branched alkanes, which enhance the octane number of gasoline, can be produced from waste polyethylene. However, achieving highly selective production of branched alkanes presents a significant challenge in the upcycling of waste polyethylene. Here, we report a one-pot process to convert polyethylene into gasoline-range hydrocarbons (C-C) with yield of 73.

Cu-Catalyzed Asymmetric Three-Component Radical Acylarylation of Vinylarenes with Aldehydes and Aryl Boronic Acids.

The direct use of readily available aldehydes as acyl radical precursors has facilitated diverse three-component acylative difunctionalization reactions of alkenes, offering a powerful route to synthesize β-branched ketones. However, asymmetric three-component acylative difunctionalization of alkenes with aldehydes still remains elusive. Here we report a copper-catalyzed asymmetric three-component radical acylarylation of vinylarenes with aldehydes and aryl boronic acids.

Potassium ion channel modulation at cancer-neural interface enhances neuronal excitability in epileptogenic glioblastoma multiforme.

The central nervous system (CNS) is increasingly recognized as a critical modulator in the oncogenesis of glioblastoma multiforme (GBM), with interactions between cancer and local neuronal circuits frequently leading to epilepsy; however, the relative contributions of these factors remain unclear. Here, we report a coordinated intratumor shift among distinct cancer subtypes within progenitor-like families of epileptic GBM patients, revealing an accumulation of oligodendrocyte progenitor (OPC)-like subpopulations at the cancer-neuron interface along with heightened electrical signaling activity in the surrounding neuronal networks. The OPC-like cells associated with epilepsy express KCND2, which encodes the voltage-gated K channel K4.

Bioaccumulation mechanisms of perfluoroalkyl substances (PFASs) in aquatic environments: Theoretical and experimental insights.

Per- and polyfluoroalkyl substances (PFASs) are persistent, bioaccumulative contaminants found in water resources at levels hazardous to human health. However, the PFAS bioaccumulation mechanism remains poorly understood. In this study, we incorporated density functional theory (DFT), molecular dynamics (MD), and experiments to analyze the partitioning pathways and to establish the structure-bioaccumulation relationship.

Iodide Ion-Promoted Highly Regioselective Triazolization of Aldehydes via Desulfonation-Associated Direct Radical Coupling.

A highly efficient iodide ion (I)-promoted method for direct α-C(sp)-H triazolization of aldehydes has been developed for the regioselective synthesis of -substituted triazole derivatives. The developed method features the corresponding products in good yields (up to 99%) with an excellent functional group tolerance via an intermolecular oxidative radical coupling. Experimental mechanistic investigations indicate that the reaction proceeds via an I-promoted synergistic desulfonylation process, which provides a high regioselectivity.

Multifunctional chiral metal hydrogen-bonded organic frameworks constructed from lanthanide ions with a trigonal prismatic coordination environment.

Two pairs of chiral enantiomers D/L-Dy(PMP)·2HO (D-1/L-1) and D/L-Yb(PMP)·2HO (D-2/L-2) were synthesized by the introduction of enantiomerically pure D/L-PMP (PMP = (phosphonomethyl)proline) ligands into lanthanide coordination chemistry. The chiral characteristics of these products were confirmed by single crystal X-ray diffraction, second harmonic generation (SHG) measurements and circular dichroism (CD) spectroscopy. These complexes are composed of 1D chains constructed from lanthanide ions with a trigonal prismatic coordination geometry and PMP ligands.