Frontiers of Chemical Science and Engineering最新文献

Dielectric barrier discharge plasma-driven dry reforming of methane is a promising technology for syngas production. However, plasma involves complex chemical reaction pathways, non-thermal equilibrium kinetic characteristics, and interactions with catalysts, which together affect the catalytic efficiency of the dielectric-barrier plasma driven dry reforming of methane reaction and constitute its main technical challenges. This study systematically investigates the effect of critical parameters-including reactor dimensions, input power, gas flow rate, gas composition, and catalyst type-on CH₄ and CO₂ conversion as well as syngas selectivity. Through thermodynamic and kinetic analysis, we elucidate the stepwise evolution mechanism of CH₄/CO₂ reactions under low-temperature plasma conditions. Notably, we incorporated the power law relationship between electron energy and input power into the thermodynamic model, thereby quantitatively revealing for the first time the regulatory effect of input power on the reaction path. This study provides valuable design principles to enhance the efficiency and industrial applicability of dielectric-barrier plasma driven dry reforming of methane processes.

Continuous-flow microwave-assisted heating has been extensively applied in chemical engineering. A common method used for heating fluids is by using a tube in a cavity. However, it is challenging to maintain high heating efficiency owing to the temperature-dependent dielectric properties of different fluids, and the temperature of fluids is usually uneven. In this study, a multilayer ring structure is proposed based on an impedance gradient that covers a tube with a porous material inside it to achieve high heating efficiency and uniformity. A multiphysics model, including electromagnetic fields, fluid heat transfer, and free and porous media flow, was established to simulate the continuous-flow microwave heating process. The dimensions of the multilayer ring structure were optimized and manufactured. Energy utilization efficiency experiments and continuous heating experiments were conducted, which demonstrated that the proposed model achieved an efficiency > 90% with different aqueous ethanol solutions, while maintaining high heating uniformity compared with other heating models. Furthermore, the effects of the tube permittivity and porosity of the porous material on the heating efficiency were investigated to demonstrate the robustness of the proposed model.

Development of ratiometric fluorescent probes for Cu²⁺ in aqueous solutions and biological systems remains the challenging task, given that Cu²⁺ commonly acts as an efficient fluorescence quencher. In this work, a novel dyad compound NI-SP bearing energy donor naphthalimide and energy acceptor styrylpyridine chromophore has been prepared using azide-alkyne click reaction. The photophysical properties of NI-SP and its coordination with Cu²⁺ have been investigated by the absorption and fluorescent spectroscopy. Upon addition of Cu²⁺ to a solution of NI-SP, the long wavelength emission peak of styrylpyridine (600 nm) was quenched, whereas the fluorescence of naphthalimide (450 nm) was enhanced due to a decrease in resonance energy transfer efficiency between the chromophores in the (NI-SP)·Cu²⁺ complex. The observed spectral changes enable ratiometric detection of Cu²⁺ by the registration of the ratio of fluorescence intensities I₄₅₀/I₆₀₀. The probe exhibited high selectivity toward Cu²⁺ in the tested conditions. The detection limit was determined at 120 nmol·L⁻¹, and the stability constant for (NI-SP)·Cu²⁺ was found to be 3.0 × 10⁶ L·mol⁻¹. Bioimaging experiments showed the NI-SP could penetrate human lung adenocarcinoma A549 cells, accumulate in mitochondria, and respond to the presence of Cu²⁺ via the changes in the fluorescence intensity of styrylpyridine fragment.

With the increasing global demand for sustainable energy and environmental solutions, the development of efficient, cost-effective, and eco-friendly electrocatalysts has become a key area of research. Microorganisms, with their distinctive microstructures, abundant functional groups, and diverse metabolic activities, offer innovative pathways for the green synthesis of electrocatalysts. This review first systematically summarizes microbial-derived electrocatalysts by using microorganisms (bacteria, fungi, viruses) as templates and metabolites, e.g., extracellular polymers, bacterial cellulose as mediates, and their applications in various representative electrocatalytic reactions, including hydrogen evolution reaction, oxygen evolution reaction, and oxygen reduction reaction. We then particularly focus on the application of microbial-derived electrocatalysts in CO₂ reduction reaction. Microorganisms not only serve as structural templates to impart high surface areas and ordered pores to catalysts but also facilitate the introduction of active sites through metabolic processes, significantly enhancing catalytic efficiency toward the optimization of reduction products. Finally, the current challenges as well as future optimization strategies are proposed in the field of microbial-derived electrocatalysts. This work offers a guideline for the design of microbial-mediated catalytic materials, advancing new strategies toward achieving carbon neutrality.

With the widespread application of 5G technology and the rapid development of electronic device miniaturization, electromagnetic radiation interference has become an increasingly critical concern. To meet the requirements of new-generation portable wearable electronic devices for electromagnetic interference shielding in terms of environmental friendliness, sustainability, lightweight, and high strength characteristics, novel shielding materials represented by carbon-based materials, MXene, and biomass materials, have emerged. To optimize the electromagnetic shielding composites for higher efficiency, researchers have proposed multifaceted strategies, including material design strategies (e.g., combinations of one-dimensional and two-dimensional materials or conductive and magnetic materials), structural design strategies (e.g., porous structures, multilayer structures, and core-shell structures), and reinforced absorption design strategies. This study provides a concise review of representative electromagnetic interference shielding raw materials, with a focus on the development status of novel biomass electromagnetic shielding materials represented by wood, lignin, and cellulose. The advantages and disadvantages of various electromagnetic shielding materials are systematically analyzed. For the first time, a summary of transdisciplinary multiscale design strategies is provided to promote the development of electromagnetic shielding techniques.

Reverse water-gas shift reaction represents a strategic pathway for CO₂ utilization. Despite its potential, reverse water-gas shift reaction via conventional thermal-catalysis faces several challenges, including low equilibrium conversion rates due to thermodynamic constraints, high energy consumption, and insufficient product selectivity. Here, this study demonstrates an evident synergetic effect between plasma and Ag/ZnO, on enhancing reverse water-gas shift reaction. The plasma catalytic system achieved significantly improved performance with a remarkable CO₂ conversion rate of 76.5%, a high CO selectivity of 96.8% and a CO yield of 74.1%, along with an energy efficiency as high as 0.19 mmol·kJ⁻¹, surpassing the plasma alone system and ZnO catalytic systems. Results from X-ray photoelectron spectroscopy and Auger electron spectroscopy confirm the presence of electronic metal-support interactions between Ag and ZnO, which facilitates the formation of electron-deficient Ag sites and partially reduced ZnO_x species. These reactive sites, along with oxygen vacancies created during reduction treatment, enhance the adsorption and activation of H₂ and CO₂, offering a dominant plasma-assisted surface reaction pathway for the improved reverse water-gas shift reaction. These findings underscore the crucial role of electronic metal-support interactions in manipulating surface environments to facilitate efficient plasma-assisted catalytic reactions, with significant implications for the rational design of catalysts capable of converting CO₂ efficiently under mild conditions.

Accurate prediction of molecular fusion properties is critical for energy-efficient material design and sustainable process optimization, yet remains challenging due to data scarcity and complex thermodynamic interdependencies. This work introduces machine learning tools to address these gaps by combining expert-curated molecular descriptors with deep learning. By systematically evaluating statistical machine learning algorithms and attention-based architectures, optimized models are identified: a SMILES-augmented Transformer-Convolutional Neural Network for fusion temperature and a graph attention network for fusion enthalpy. Prediction power is further validated experimentally on four structure diverse compounds (γ-butyrolactone, methyl octanoate, N-phenylbenzenesulfonamide, and triethylene glycol dimethyl ether). Interpretability analyses reveal that these models prioritize key structures in molecules: attention in text-based models focuses on key atoms while that in graph models focuses on key chemical bonds, aligning with empirical thermodynamic evidences. By providing rapid, interpretable fusion property predictions, this framework can support the development of low-energy phase-change materials and sustainable solvent systems, advancing data-driven green chemistry.

Surface-grafted polymer brushes with controlled properties and nanoscale thickness are ideal candidates for transparent coatings to prevent biofouling. However, maintaining long-term antibacterial performance in natural environments remains a significant challenge. In this study, we present a metalated polymer brush (Mt-PB) coating that combines excellent transparency with antimicrobial properties. The coating is prepared by incorporating transition metal ions (e.g., Cu and Ag) into surface-grafted polymer brushes through cooperative in situ reduction. Due to the ultra-thinness of the metalated brush layer (Cu-PB, ∼60.07 nm; Ag-PB, ∼57.45 nm), the resulting coating exhibits high optical transmittance (∼86%) and superior antibacterial efficiency (∼99.99% inhibition rate against E. coli and S. aureus). Additionally, the Mt-PB-coated lens demonstrates excellent antibacterial and antifouling durability, as evidenced by underwater detection tests that provide high-resolution images and stable transparency (Δ < 2%) for over a month of underwater exposure. These findings offer a promising strategy for developing transparent and antifouling coatings suitable for underwater optical devices.

The persistent presence of levofloxacin (LEV) residues in aquatic environments considerably threatens ecological safety and human health, owing to the potential spread of microbial resistance genes, creating an urgent need for effective removal technologies. In this study, porous carbon materials with high specific surface areas were synthesized using a one-step KOH activation method, with medium-low-temperature coal tar pitch serving as a carbon precursor. In addition, the performance and mechanism of LEV degradation via peroxydisulfate (PDS) activation were systematically explored. Characterization techniques such as X-ray diffraction, Raman spectroscopy, N₂ adsorption-desorption analysis, and field-emission scanning electron microscopy revealed that K11 possessed abundant pores, a specific surface area of up to 1220 m²·g⁻¹, and numerous defects, which collectively provided a structural basis for its catalytic activity. Degradation experiments demonstrated that the LEV removal rate exceeded 91% under conditions of a 0.2 g·L⁻¹ PDS dosage, a 0.1 g·L⁻¹ K11 dosage, pH levels ranging from 3 to 9, and a temperature of 30 °C, with robust resistance to interference from co-existing ions and humic acid. Even in real water bodies, a removal rate of over 77.84% was maintained. Free-radical quenching experiments and electron spin resonance assays confirmed that the reaction proceeded predominantly via non-radical pathways, primarily involving the generation of singlet oxygen by PDS, along with a minor contribution from direct electron transfer pathways. High-performance liquid chromatography-mass spectrometry identified LEV degradation intermediates, suggesting that the degradation pathways include piperazine ring cleavage, defluorination, and oxidation of the quinolone backbone. This study offers theoretical insights and technical guidance for the resource utilization of coal tar pitch and the control of antibiotic pollution.