Latest ArticlesSingle-atom catalysts (SACs), especially defective-SACs, have been developed into low-cost, high-selectivity and high-performance advanced catalysts due to their unique synergistic effects, and have occupied a place in the energy and environmental fields. However, there is a lack of comprehensive and comprehensive summaries and discussions on the structure-property relationships. Therefore, an exhaustive review on the topic of the synergistic interaction of SACs with defective catalysts is imminent. Firstly, this review offers an overview of the most recent generation pathways of defective-SACs based on SACs and defect formation time differences, with a focus on the important influencing factors in the different synthesis processes. Immediately thereafter, the different roles of defects in the constructed defective-SACs are comprehensively analyzed to unravel the mystery of the high stability and performance of defective-SACs. Subsequently, this article systematically analyzes the synergistic interaction mechanism between defects and SACs from the perspective of reaction mechanisms and explains how this mechanism drives significant performance improvements in various catalytic reactions. The article concludes with limitations of current research and future directions to guide the design of more perfect catalysts for defective-SACs.
The heterogeneous electro-Fenton (HEF) technology is a promising yet challenging approach for organic pollutant degradation. It is urgent to develop a catalyst for both highly efficient H2O2 and hydroxyl radical (•OH) generation with low energy consumption at neutral conditions. This study presents a bifunctional catalyst (CoPc/OCNTs/FeOF) synthesized by ultrasonic anchoring of FeOF onto cobalt phthalocyanine-modified oxidized carbon nanotubes. The catalyst demonstrated synergistic effects, achieving a 2.94-fold enhancement in H2O2 generation and a 3.85-fold increase in •OH yield compared to its individual components (CoPc/OCNTs and FeOF). At pH 6, the CoPc/OCNTs/FeOF cathode enabled nearly complete phenol removal within 90 min, with a high kinetic rate constant (k) of 0.04848 min-1, driven by cooperative oxidation from singlet oxygen (1O2) and •OH. The system exhibited exceptional stability, inorganic ion tolerance, and broad applicability to real wastewaters, achieving 82.0% total organic carbon (TOC) removal for phenol wastewater at a low energy consumption of 21.9 kWh kg-1 COD-1. Moreover, sodium alginate-immobilized microalgae hydrogel was integrated into the HEF system to supply O2 in situ for the 2e- oxygen reduction reaction (ORR), eliminating energy-intensive mechanical aeration. Subsequent microalgal cultivation further removed 90.6% of total nitrogen and 82.8% of total phosphorus, showcasing a sustainable dual-function strategy for pollutant degradation and nutrient recovery. This work advances the design of efficient HEF catalysts and highlights the potential of microalgae-coupled systems for sustainable wastewater treatment.
Micro/nanoplastics (MNPs) have emerged as a global environmental concern, which leads to an urgent need for sensitive and specific MNPs detection technologies. Fluorescence-based methods with high sensitivity and dynamic tracking capabilities have become a significant and promising tool in MNPs analysis. This review systematically summarizes recent developments in fluorescent probes including traditional organic dyes, nanomaterials, aggregation-induced emission (AIE) molecules, binding peptides, and aptamers, for MNPs detection. The fluorescence sensing technology coupled with micro-imaging developed for in situ detection and dynamic tracking is also discussed. The current challenges for MNPs detection including matrix interference and lack of quantification standards are discussed and perspectives including developing multifunctional probes and AI-assisted platforms are proposed. This review provides theoretical reference and innovative ideas for developing new fluorescence probes and methods for MNPs detection and monitoring.
To reduce the pollution of waste heat to the environment and achieve Sustainable Development Goals, recovering and utilizing of low-grade heat is critical. Although various thermal conversion technologies have been extensively developed, research on thermal energy storage materials with dynamically adjustable properties for diverse applications is still lacking. Herein, hydrated salt hydrogel with switchable stiffness and tunable thermal performance was fabricated by simply incorporating sodium acetate trihydrate into hydrogel network. Hydrated salt hydrogel displayed adjustable thermal performance (maximum heat release temperature from 53 ℃ to 20 ℃; enthalpy value from 0 to 179 J/g) by regulated sodium acetate trihydrate concentration of hydrogels. Moreover, the control of variable mechanical strength (0.03–5.21 MPa) and toughness (0.02–420.58 MPa) was accomplished. The study further demonstrates the promising application of hydrated salt hydrogel in thermal management for electronics and controllable soft-rigid coupling thermoelectric devices, opening new opportunities in waste heat recovery and achieving Sustainable Development Goals.
Alkaline anion exchange membrane water electrolysis (AEMWE) is a low-cost and sustainable technology for hydrogen production. This study presents the development of high-performance anion exchange membrane (AEM) and ionomers based on quaternized poly(diphenyl carbazole) with rigid ether-bond-free aryl backbone and flexible multination strings in the side chains. The optimized molecular architecture induces pronounced microphase separation, enabling high hydroxide conductivity (159.3 mS/cm at 80 ℃) and exceptional alkaline stability (1 mol/L KOH at 80 ℃, retains 97.5% ionic conductivity and 88.6% tensile strength after 1800 h). By implementing an anode water-fed/cathode water-free configuration and regulating the structure and content of ionomers at anode and cathode electrodes, the AEMWE performance was significantly improved from 1.9 A/cm2 to 4.2 A/cm2 at 2 V (a 2.2-fold increase) using 1 mol/L KOH solution as the electrolyte. Under pure water conditions, the electrolyzer still achieved an excellent electrolysis performance of 1.8 A/cm2 at 2 V. Furthermore, the fabricated AEMWE exhibited an outstanding in-situ durability with a low voltage degradation rate of 0.17 mV/h during a continuous operation of 1185 h at a current density of 0.5 A/cm2.
Mass spectrometry is a highly sensitive and precise analytical technique widely utilized in biomedical research, drug development, and environmental monitoring. Nonetheless, before mass spectrometry analysis, complex matrix samples frequently harbor numerous salts, which may compromise the stability and accuracy of mass spectrometry signals. Hence, it is imperative to employ effective desalting techniques, which serve as critical pretreatment steps in sample preparation for mass spectrometry analysis. While numerous scholars have developed desalting techniques, a comprehensive overview of such techniques is lacking. This paper provides a summary of desalination methods for mass spectrometry analysis developed since the twenty-first century (including extraction techniques, chromatography, ion exchange, crystallography, ambient ionization mass spectrometry and desalting agents, etc.), along with their principles, advantages, and disadvantages. Furthermore, recent research advancements and technological enhancements are discussed to introduce novel ideas and methodologies for sample desalting as a pretreatment step before mass spectrometry analysis. Against the backdrop of the growing importance of precision medicine and environmental monitoring, the continuous improvement of desalination technology will promote its wide application in areas such as clinical diagnosis, food safety testing, and environmental pollution assessment.
The treatment of nitrogen-contained refractory organic wastewater faces challenges due to complex composition and high toxicity. While microscale zero-valent iron (mZVI) based processes enable simultaneous removal of organic contaminants and nitrate (NO3−-N), electron competition and excessive iron sludge generation limit efficiency. This study reveals the dual roles of NO3−-N in the mZVI/O2 process: Inhibiting the oxidative removal of organic contaminants through electron competition and simultaneously enhancing iron dissolution with TFe increased by 17.5% to 65.7% compared to the system without NO3−-N. Nitrogen conversion analysis indicates that NO3−-N is mainly converted to NH4+-N via a direct 8-electron reduction pathway. To increase the utilization efficiency of iron electrons and enhance organic contaminant removal, a two-stage gradient oxidation process (mZVI/O2-Fenton) is designed: 1st stage utilizes NO3−-N to enhance Fe0 corrosion for NO3−-N reduction and Fe(II) release, while 2nd stage achieves efficient organic contaminants degradation via Fenton reaction with addition of H2O2. Actual wastewater validation confirms synergistic high organic contaminants removal (COD removal > 79.5%) and targeted nitrogen conversion (> 66.4% NO3−-N to NH4+-N). The study overcomes electron competition limitations in the mZVI/O2 process and provides a synergistic pollution control-resource recovery strategy for NO3−-N-contained refractory organic wastewaters.
In situ chemical oxidation (ISCO) technology using peroxymonosulfate (PMS) and natural iron-bearing minerals for groundwater remediation has received increasing interest. The interaction between PMS and active Fe sites in minerals significantly influences the effectiveness of groundwater remediation. Nevertheless, there has been limited research investigating the relationship between the minerals active Fe sites and PMS activation. Herein, we distinguished and quantified the active Fe sites of common natural iron-bearing minerals in groundwater aquifers. Lewis acid sites (Fe-OH) were confirmed as the reaction sites in iron oxide/hydroxide/bearing clay minerals. The activation performance of minerals is positively correlated with their Lewis acid content. In iron sulfide minerals, Fe-S sites act as electron transfer mediators, facilitating PMS adsorption and activation. The activation of PMS by Lewis acid and Fe-S sites free radical both led to the generation of free radicals (SO4·- and ·OH) for CPs removal. Moreover, typical ferrihydrite/PMS and pyrite/PMS systems exhibited resistance to environmental interference and broad pH adaptability. A one-dimensional sand column experiment further proved their feasibility and long-term applicability in saturated porous media. These findings highlight the critical influence of active Fe sites of natural iron-bearing minerals and provide technical support for the application of PMS-ISCO strategies for groundwater remediation.
This study presents a OH− concentration-regulated one-step hydrothermal synthesis of a novel SrBi4Ti4O15/BiOCl heterojunction for efficient antibiotic degradation. Precise control of alkaline conditions enabled the in-situ generation of Ti–Cl bonds at the heterointerface, with their presence and nature further corroborated by Raman and XPS analyses. The SBTO/BOC heterojunction demonstrated significantly enhanced charge separation, achieving a 91.5% tetracycline degradation rate under illumination, outperforming pure BiOCl (71.9%) and SBTO (54.8%). Radical trapping and EPR studies identified •O2− and •OH as the primary reactive species. The catalyst exhibited robust stability, broad pH tolerance, and resistance to ionic interference. Tetracycline degradation efficiency further improves under combined light and ultrasonic irradiation, leveraging piezoelectric polarization to boost charge separation. LC-MS analysis revealed reduced toxicity of degradation intermediates. This work highlights the strategic role of OH−-mediated interface engineering in designing efficient ferroelectric heterojunctions for wastewater remediation.
Iron oxide based magnetic catalytic colorimetric (MCC) nanomaterials have attracted extensive attention as signal labels in lateral flow immunoassays (LFIA). However, the main challenge in this field is its weak catalytic activity leading to relatively low color intensity. Herein, a new strategy of using the metal-organic framework (MOF) as mediate interfacing layer for loading Pt nanoparticles (Pt NPs) on the magnetic nanoparticles (MNPs) was proposed to obtain MCC nanomaterials with high catalytic activity. First, Cu-Co MOF was grown in situ with MNPs as the core, and then the MOF interfacing layer facilitates the uniform growth of Pt NPs on it. The obtained MNPs@MOF@Pt nanocomposite exhibited enhanced color signal intensity, excellent peroxidase-like activity and strong magnetic separation ability. After integration with a dual-antibody sandwich LFIA platform, the highly sensitive detection of interleukin-6 was achieved with a detection limit of 8.3 and 2.8 pg/mL for the pre-catalytic and post-catalytic tests respectively, which were 58-fold and 171-fold higher than that of the LFIA based on gold nanoparticles. Moreover, it exhibited good specificity and high accuracy for detection of clinical serum samples. Therefore, the magnetic nanozyme material proposed in this study demonstrated great potential for application in point-of-care diseases diagnosis.
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