RSC Advances最新文献

Electrodes are crucial for electrochemical supercapacitor performance, and thin-film electrodes with active layers on conductive substrates enable fast ion transport and efficient charge storage, making them ideal for advanced supercapacitor applications. However, achieving high areal capacitance on titanium current collectors with a simple, binder-free process remains challenging. In this work, we fabricate a binder-free PANI-Ni-Co hybrid film on Ti sheets by sequential electrodeposition of a Ni-Co alloy followed by in situ electrochemical polymerization of polyaniline. XRD, SEM/EDS, and XPS confirm a finely granular Ni-Co scaffold conformally coated by a porous PANI overlayer. Compared with bare Ti and Ni-Co/Ti, the PANI-Ni-Co/Ti electrode exhibits markedly enhanced charge storage in 1.0 M H₂SO₄. It delivers an areal capacitance of 1230 mF cm^-2 at 1 mA cm^-2 from GCD and 2819 mF cm^-2 at 5 mV s^-1 from CV, while retaining 272.5 mF cm^-2 at 10 mA cm^-2 and ∼11% of its low-rate capacitance at 200 mV s^-1. Notably, the electrode shows good cycling durability, retaining 81.8% of its initial capacitance after 1000 GCD cycles, and post-cycling CV profiles recorded in the used and refreshed electrolytes remain essentially unchanged, indicating preserved electrochemical integrity. The Ragone analysis shows energy densities up to 0.11 mWh cm^-2 at 0.4 mW cm^-2, decreasing to 0.025 mWh cm^-2 at 4.0 mW cm^-2. EIS reveals reduced solution and charge-transfer resistances and near-ideal capacitive behavior for the hybrid electrode. This simple, room temperature, all electrochemical strategy provides a scalable route to high-areal-capacitance Ti-based electrodes for miniaturized supercapacitors, which are suitable for powering or buffering low-power wearable and microelectronic devices.

This work presents a first-principles investigation of the mixed-anion perovskite Sr₃NF₃, evaluating its photocatalytic potential under biaxial strain. Stability analysis confirms its structural, dynamic and mechanical robustness. Sr₃NF₃ exhibits a direct bandgap of 2.06 eV (HSE06), tunable from 1.77 eV under +6% tensile strain to 2.16 eV under -6% compressive strain. Electron density difference plots reveal strong internal charge separation attributed to the mixed-anion framework. Optical results show that Sr₃NF₃ exhibits high absorption in both visible and UV regions, with compressive strain enhancing absorption (∼1.35 × 10⁵ cm^-1) and the static dielectric constant (ε = 4.11), improving carrier separation. While unsuitable for hydrogen evolution, Sr₃NF₃ shows strong intrinsic oxidation driving force for oxygen evolution, exhibiting an overpotential of 1.51 eV at -6% strain. Low carrier effective masses further suggest fast charge transport. These findings identify Sr₃NF₃ as a promising, strain-tunable mixed-anion perovskite with favorable intrinsic electronic properties for oxygen evolution, and suitable as an OER-oriented component in advanced photocatalytic architectures.

The growing occurrence of pharmaceutical contaminants in aquatic systems has intensified the demand for advanced nanostructured materials capable of selective adsorption and removal of such pollutants. Paracetamol, a commonly used analgesic and antipyretic drug, is frequently detected in wastewater and poses severe ecological and health risks when accumulated in the water bodies and the soil. In this study, density functional theory (DFT) calculations were employed to investigate the structural, electronic, and adsorption behaviors of phosphorus (P), sulfur (S), and silicon (Si) doped COF-PEDOT frameworks for paracetamol adsorption. All geometries were optimized using the PBE0-D3/6-311G(d) basis set. The optimized structures exhibited minimal distortion after adsorption, indicating stable interactions between the adsorbate and the doped surfaces. Density of states (DOS) analysis revealed that heteroatom incorporation enhanced the electronic activity and reactivity of the complexes, while frontier molecular orbital (FMO) analysis showed a notable narrowing of the energy gap, confirming improved electron transfer capability. The ionization potential values (5.29-5.44 eV) remained within the range of moderately stable adsorbents. Natural bond orbital (NBO) analysis indicated that phosphorus doping produced the highest orbital stabilization energies, suggesting stronger donor-acceptor interactions. Adsorption energy calculations yielded negative values for all systems, confirming exothermic and thermodynamically favorable adsorption processes. Furthermore, quantum theory of atoms in molecules (QTAIM) and non-covalent interaction (NCI) analyses demonstrated the presence of weak but stable van der Waals and hydrogen-bond interactions governing paracetamol adsorption. The results demonstrate that tailored heteroatom doping can effectively tune the electronic and adsorption characteristics of COF-PEDOT frameworks. The P-, S-, and Si-doped systems exhibit enhanced sensitivity, stability, and reversibility, making them promising candidates for the selective adsorption of paracetamol from pharmaceutical contaminants in aquatic environments.

[This corrects the article DOI: 10.1039/D5RA08944A.].

Loganin is an active compound derived from Cornus officinalis Sieb. et Zucc., which has been widely used due to its excellent pharmacological effects including anti-diabetic, anti-inflammatory, neuroprotective, and anti-tumor properties. However, the metabolic process of loganin in vivo is insufficiently elucidated until now. Therefore, a metabolic networking cluster combined with multiple data processing techniques based on UHPLC-MS was applied to predict the metabolites of loganin and explore their temporal dynamic change patterns. First, the target ions in the blank and dosed groups were systematically screened using the Compound Discoverer (CD) software. Then, the potential metabolites were identified based on the workflow of CD. Second, a metabolic networking cluster (MNC) was proposed to predict the metabolites of loganin according to the related reports in the literature and existing metabolites of loganin. Third, the establishment of diagnostic product ions (DPIs) was used to preliminarily screen and identify the potential metabolites of loganin. As a result, 2 critical metabolites, including loganin and loganetin, were proposed as networking cluster cores, and a total of 34 metabolites were screened and characterized. Results indicated that loganin primarily underwent the deglucosylation, glucuronidation, demethylation, sulfation, and dehydroxylation reactions and their composite reactions in vivo. In addition, most metabolites reached their peak concentration between 0.5 and 1 h and then gradually decreased, indicating that the metabolic process of loganin in rats was relatively rapid. In summary, an integrated strategy was proposed to comprehensively elucidate the metabolic pathways of loganin in vivo, which provides a vital reference for research on the metabolism of other compounds.

This review highlights recent advancements in the preparation and environmental applications of functionalized adsorbent hydrogels, with a focus on their role in addressing global water pollution and scarcity. Hydrogels, with their unique three-dimensional crosslinked structures and exceptional water retention capabilities, have emerged as versatile materials for water purification. The review encompasses various synthesis methods, including chemical cross-linking and radiation-induced polymerization, and examines their mechanisms for pollutant removal, including adsorption, ion exchange, electrostatic interactions, and photocatalytic degradation. Additionally, integrating nanomaterials into hydrogels enhances their mechanical properties and contaminant-removal efficiency. The review also discusses innovative applications, including solar-driven water remediation, microbial inactivation, and simultaneous water and power generation. These advancements position hydrogels as sustainable and efficient solutions for global water security challenges.

Challenges in heavy oil bioupgrading necessitate innovative approaches. Hence, we delved into the simultaneous application of a bacterium (Geobacillus stearothermophilus) and Al₂O₃ nanoparticles for heavy oil upgrading at a high temperature. We used the central composite design method within Design Expert software. The initial oil volume, upgrading time, and nanoparticle concentration were the main variables. Aromatic/aliphatic content and oil viscosity were the two independent responses. Results showed that nanoparticles could have accelerated bioupgrading. The zeta potential, FESEM and EDS confirmed the absorption of nano alumina on the bacterial cell due to the formed ion-dipole interaction between alumina and bacterial cells, which could have intensified the entry of heavy oil molecules into the bacterial cell. The best outcomes were observed during 11.86 days, with 26% v/v initial oil and 0.46% W nanoparticles, as indicated by FTIR spectroscopy, which showed a reduction in the aromatic/aliphatic index from 0.29613 to 0.07677 and a decrease in oil viscosity from 480 cp to 144 cp. Moreover, as determined by GC-MS, a remarkable 100% decrease in certain cyclo compounds and a considerable improvement in upgrading efficiencies for some contents such as cyclohexanes were observed. Also, a 14% decrease in asphaltene content was associated with a decrease in the solo use of bacteria. These findings highlight the synergistic efficacy of G. stearothermophilus and alumina in upgrading heavy oil.

In this work, we explore the possibility of applying automated crystal structure prediction to reproduce the experimentally identified metastable porous polymorphs. Using our recently developed High-Throughput Organic Crystal Structure Prediction () framework, we conducted a systematic study on five representative organic crystalline systems including hydrogen-bonded frameworks (HOFs), featured by the presence of significant porosity, in conjunction with different choices of energy models from classical, machine learning force fields, tight binding to density functional theory. Our results suggest that the current structure generation framework, with careful selection of symmetry conditions, is likely to generate rather complex and abundant metastable crystal candidates for porous crystals. In conjunction with the recent advance in universal machine learning force fields, it becomes possible to identify experimental structures as the energetically favorable candidates from a simple energy versus density analysis, thus paving the way for computational design of complex porous materials with the target systems prior to the experimental synthesis and characterization.

The disposal of coal gasification fine slag (CGFS) and the treatment of dye wastewater present substantial environmental pressures. Therefore, developing cost-effective adsorbents is crucial. In this study, CGFS-based adsorbents, which are modified with dimethyl diethoxy silane (DDS-CGFS) and dodecyl trimethyl ammonium chloride (DTAC-CGFS), were prepared and applied for the removal of rhodamine B (RhB) organic dye. The adsorption performances were evaluated across different pH values, temperatures, and contact time. Under optimal conditions (pH = 7, 328.15 K, 24 h), the DDS-CGFS adsorbent exhibited a maximum adsorption capacity of 92.82 mg g^-1 for rhodamine B. Kinetic and isotherm analyses revealed that the adsorption involved both physical and chemical processes. The intra-particle diffusion model suggested that the adsorption kinetics were governed by boundary-layer and intra-particle diffusions. Thermodynamic parameters (ΔG° < 0, ΔH° > 0, ΔS° > 0) indicated that the adsorption was a spontaneous and endothermic process accompanied by an increase in entropy. Material characterization and model fitting suggested a synergistic adsorption mechanism, potentially involving interactions such as hydrogen bonding and π-π stacking. Overall, DDS-CGFS and DTAC-CGFS are low-cost adsorbents for remediating dye wastewater. Due to their outstanding adsorption capacity, they show potential as ideal adsorbents for dye wastewater treatment.

In this study, we report a streamlined one-pot synthesis of a new series of (E)-4-phenyl-2-(2-(pyren-1-ylmethylene)hydrazinyl)thiazole derivatives (4a-4o). The reaction involves the condensation of pyrene-1-carbaldehyde, thiosemicarbazide, and α-halo ketones in the presence of a catalytic amount of InCl₃ as a Lewis acid catalyst, carried out under reflux in a (1 : 1, v/v) H₂O/EtOH medium at 80 °C. This protocol provides several key advantages, including mild reaction conditions, short reaction times, excellent yields, broad functional group tolerance, and the added benefit of chromatography-free product isolation, thereby enhancing practicality and operational simplicity. All synthesized compounds were fully characterized using ¹H NMR, ¹³C NMR, FT-IR spectroscopy, and LC-MS analysis. The anticancer potential of the synthesized derivatives was evaluated against the human breast cancer cell line (MCF-7) using an in vitro MTT assay. Compounds 4m and 4g exhibited the most promising cytotoxic effects, displaying IC₅₀ values of 43.66 and 45.24 µg mL^-1, respectively. Furthermore, molecular docking studies were performed to elucidate structure-activity relationships, revealing a strong correlation between the predicted binding affinities and the experimental biological outcomes.