Latest ArticlesThe Fenton-like activation of peroxymonosulfate (PMS) is an effective oxidation strategy for water decontamination, however, Fe(Ⅱ)-mediated Fenton-like reactions suffer from limitations of sluggish iron species cycling and iron sludge accumulation. Herein, molybdenum pentaboride (Mo2B5) was innovatively employed as a dual-functional co-catalyst to address these challenges via synergistically direct and indirect routes for activating PMS. Mo2B5 can promptly enhance Fe(Ⅲ)/PMS to entirely degrade sulfamethoxazole within 4 min, superior to conventional reducing agents and carbon-based co-catalysts. Based on mechanism investigations (reactive oxygen species analysis, iron species variation, surface chemistry characterizations), the distinctive electronic configuration of Mo2B5 can direct activate PMS for generating hydroxyl radical (•OH), while simultaneously enhance Fe(Ⅱ) regeneration to facilitate subsequent Fenton-like processes to produce sulfate radicals (SO4•−) and ferryl species (Fe(Ⅳ)). The system thus demonstrated broad applicability for degrading diverse pollutants with high rate constants, while the substrate specific reactivities are dependent on the electron-donating capacities of pollutants. In addition, Mo2B5 exhibits exceptional stability over consecutive cycle tests, attributed to its self-cleaning surface and retained crystallinity.
Most bioactive compounds (amino acids, sugars, peptides, proteins) and drugs are chiral. Although the enantiomers have similar physical and chemical properties, they may exhibit completely different physiological effects in terms of biological activity, toxicity, and pharmacological effects. Therefore, chiral recognition is particularly important in numerous fields. Surface-enhanced Raman scattering (SERS) spectroscopy, a promising nondestructive analytical technique with wide applications in biosensing, food safety, and environmental analysis, exhibits exceptional potential for chiral recognition. However, there remains a notable scarcity of comprehensive reviews focusing on SERS-based chiral recognition. This review introduced the development of SERS and summarized the classification of chiral enantiomers recognition by SERS spectroscopy in detail in the past 10 years, mainly including EM-dominated chiral substrates, chiral ligand-modified systems, charge transfer (CT)-based "chiral-label-free" approaches, and chiral molecularly imprinted strategies. In addition, the potential challenges and prospects in SERS spectroscopy for chiral recognition are proposed, which is expected to effectively guide future research.
The integration of advanced sensing materials as channel layers in devices is essential for constructing field-effect transistor (FET) biosensors. In this study, we synthesized high-crystallinity bimetallic M3(hexaaminotriphenylene)2 (M = Co, Ni) thin films as FET channel materials via an in-situ growth method using a mixed solvent system of water and N,N-dimethylformamide (DMF). This bimetallic metal-organic framework (MOF)-based FET then served as a glucose biosensor, achieving a high sensitivity and an ultra-wide detection range from 10 nmol/L to 10 mmol/L. Further studies reveal that the success of in-situ growth of the high-crystalline bimetallic MOF film can be attributed to the coordination solvent exchange reaction between the metal atomic center, DMF, and water. Furthermore, the introduction of bimetallic centers enhances the number of active sites within the MOF, thereby achieving an ultra-low detection limit and an ultra-wide detection range. This work presents a versatile approach for constructing high performance FET biosensors.
Electrocatalysis stands as a cornerstone in the pursuit of clean energy conversion and environmental sustainability, with single-atom catalysts (SACs) emerging as a transformative paradigm for enhancing electrocatalytic efficiency. In the architectural design of SACs, supports transcend conventional roles as mere supports, actively governing catalytic performance via robust metal-support interactions (SMSI). This review comprehensively analyses the key role of support engineering in modulating SACs performance. The study begins with a systematic assessment of currently popular SACs synthesis strategies, critically comparing their advantages and limitations. Through a hierarchical analysis, it reveals the impact of various support materials, such as carbon-based materials, metal oxides, MXenes, and metal-organic frameworks (MOFs), on the catalytic performance of SACs, with emphasis on their structural characteristics, electronic properties, and interaction mechanisms with active sites. The review further explores applications in energy conversion/storage and environmental remediation, while addressing current challenges and proposing future research directions for SACs development. By providing actionable insights, this work aims to guide the design of next-generation SACs and advance sustainable electrocatalysis.
Elucidating the synergistic influence mechanism of catalysts composition and pollutants structure on the treatment system is a necessary way to further expand the application potential of heterogeneous iron-based Fenton-like technology in the field of water treatment from catalytic source and degradation end. In this study, a nitrogen-doped iron-carbon material (Fe-NC-4%) was synthesized to effectively activate peroxymonosulfate (PMS) to remove different organic pollutants, thus further exploring the synergistic effects of material and pollutant structures on degradation performance and mechanism. A combination of characterization analysis, experimental demonstration and density functional theory calculation showed that the more graphitic nitrogen in Fe-NC-4% assisted the Fe active centers to adsorb PMS more easily and further form the Fe-NC-4%-PMS* complex with high activity and stability. And the Fe-NC-4%-PMS* complex could efficiently and selectively degraded electron-donating organics by electron transfer process (ETP). The degradation rate of ofloxacin (OFL) with stronger electron-donating ability could reach 0.405 min−1 in the Fe-NC-4%/PMS system. In addition, the Fe-NC-4%/PMS system possessed strong environmental adaptability, safety and practical application potential. This study would provide technical and theoretical guidance for the top-down analysis of specific reaction mechanisms in Fenton-like systems, including catalyst structure design, reactive species generation and selective pollutant degradation.
Lithium–sulfur (Li–S) batteries with the high theoretical capacity of 1675 mAh/g have attracted attention as next-generation energy storage systems. Understanding the dynamic evolution and reaction mechanisms at the interface between sulfur cathodes and the electrolyte is crucial to achieve a high reversible capacity of Li−S batteries. However, due to the challenges in probing the complex Li–S redox reaction, the structural and morphological changes from active sulfur to insoluble lithium sulfide (Li2S) under operating conditions remain poorly understood. Here, the behaviors during sulfur dissolution and Li2S deposition/decomposition under realistic conditions were investigated via in situ atomic force microscopy (AFM). Direct visualizations revealed that tightly stacked sulfur particles hinder essential electronic pathways within the cathode. Furthermore constructing a conductive framework promotes more uniform Li2S deposition, which was previously dispersed across the electrode surface, thus accelerating Li2S conversion kinetics during the subsequent charge process. PeakForce tunneling atomic force microscopy (TUNA) measurements effectively elucidated the correlation between nanoscale structural features and electrical conductivity under varying potentials. Real-time observations reveal the dynamic evolution and reaction mechanisms of sulfur cathodes, offering profound insights into the Li−S redox processes and guiding the rational design of advanced cathodes.
Flexible gas sensors show promise in wearable health monitoring and toxic gas detection due to mechanical flexibility and system integration, but they still face challenges such as slow response/recovery dynamics and poor stability. Here, a novel aqueous ink consisting of n-type mesoporous tin oxide (mSnO2) colloids and p-type poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (abbreviated as PEDOT:PSS) was designed and deposited on oxygen plasma treated polyimine (PI) substrate with pre-printed electrodes and heater via automatic dispension printing followed with a subsequent freeze-drying treatment, resuling in hierarchically porous sensing layer with mesopore channels and macroporous framework on the flexible PI substrate. The resultant SnO2/PEDOT:PSS sensor showed excellent sensing performance (6%-30.5%) toward low-concentration ammonia (1–100 ppm), rapid response/recovery speed (61 s/25 s) and superior mechanical stability. Furthermore, the sensor was integrated into a Bluetooth-enabled smart bracelet, achieving real-time monitoring of environmetal ammonia concentration and showcasing its potential for wearable electronics in dectecting volatile harmful gases.
The exposure of specific facets in catalysts plays a pivotal role in surface/interface reactions. This study systematically explores facet engineering as a novel approach to enhancing the piezoelectric and piezo-photocatalytic capabilities of metal-organic frameworks (MOFs), with a focus on ZIF-8 as a model compound. By selectively exposing specific facets-(100), (110), and a combination of both in mixed configurations, this research examines how facet orientation affects piezoelectric properties, charge separation efficiency, and catalytic performance. The ZIF-8 samples, identified as ZIF-8-RD, ZIF-8-CUBE, ZIF-8-TRD1, and ZIF-8-TRD2 demonstrated distinct catalytic activities in photocatalysis, piezocatalysis, and piezo-photocatalysis. Notably, ZIF-8-TRDs, with the mixed-facet exposure, showed superior catalytic performance, achieving up to 94% degradation of tetracycline (TC) in piezo-photocatalysis, a substantial improvement over the single-facet variant. This enhanced performance is attributed to the mixed facets' higher carrier concentration and superior charge separation facilitated by the increased internal piezoelectric potential. Density functional theory (DFT) calculations corroborate the experimental results, revealing that mixed facets contribute to a larger dipole moment, indicating greater structural asymmetry and piezoelectric efficiency. The findings underscore facet engineering as an effective strategy to optimize MOF-based catalysts, opening avenues for high-performance materials tailored for environmental remediation and sustainable energy applications. This work not only pioneers facet engineering in MOF piezo-photocatalysts but also opens new avenues for the development and enhancement of high-performance MOF in piezoelectricity.
With the continuous detection of new pollutants in the water environment, their potential harm cannot be ignored. In order to explore an effective method to remove contaminants from wastewater, this paper presents an underwater bubble plasma (UBP) activated peroxymonosulfate (PMS) strategy for rapidly degrading the typical emerging contaminant tetracycline hydrochloride (TC) in water. The results indicate that, compared with UBP alone (41.1%), the UBP-PMS system (98.6%) exhibits significantly enhanced degradation ability, achieving a 57.5% increase in TC degradation rate under identical conditions while enabling long-term self-purification of wastewater without energy input within this system. In addition, we studied the effects of initial TC concentration, the type of working gas, the initial pH value of the solution, and the water matrix on the degradation performance of the UBP-PMS system. The anti-interference performance of the UBP-PMS system is proven to be strong, as six inorganic anions (HCO3−, CO32−, NO3−, HPO42−, SO42− and Cl−) are added respectively to simulate the actual water environment. The contribution of different reactive species to the degradation process was evaluated qualitatively and quantitatively by electron spin resonance (ESR) and scavenger experiments, of which the largest contribution was •OH, followed by 1O2, ONOOH/O2•-, SO4•‒ and hydrated electrons. The potential degradation pathways of TC were analyzed, and the toxicity of the degradation intermediates was evaluated by quantitative structure-activity relationship (QSAR) analysis, revealing a gradual reduction in TC toxicity under the co-treatment of UBP-PMS. This study provides a novel activation strategy involving UBP-PMS and provides valuable insights into the degradation properties and mechanisms of emerging pollutants in actual water bodies.
Sustainable and efficient solutions are essential to address increasingly critical environmental issues, particularly in the field of pollutant removal and resource recovery. The latest research has shown that pulsed electrochemistry significantly contributes to these goals by precisely altering the local reaction environment, accelerating the reaction kinetics and decreasing the overall energy requirements. However, knowledge gaps exist in dynamic evolution mechanism of electric double layer (EDL) in this technology, and challenges remain toward fully implementation of this promising technology. In this review, the fundamentals of pulsed electrochemistry and its connection to the theoretical models of EDL are comprehensively presented. The critical parameters (e.g., duty ratio, frequency and waveform) for boosting the performance of the system are systematically discussed and the typical electrochemical reactions that occur with pulsed electrochemistry are outlined. The proposed pulsed electrochemistry methodologies tailored for environmental applications are also reviewed in detail. Finally, future opportunities and challenges of this promising but fledgling field are discussed, with the expectation that this technology offers a route to transform conventional chemical industries into cleaner and more sustainable production.
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