Single-atom catalysts (SACs) have been increasingly acknowledged for their performance in sustainable Fenton-like catalysis. However, SACs face a trade-off between activity and stability in peroxymonosulfate (PMS)-based systems. Herein, we design a nano-island encapsulated single cobalt atom (Co-ZnO) catalyst to enhance the activity and stability of PMS activation for contaminant degradation via an "island-sea" synergistic effect.
View Article and Find Full Text PDFThe relentless depletion of fossil fuels accentuates the urgent necessity for the sustainable synthesis of chemicals from renewable biomass. 5-Hydroxymethylfurfural (HMF), extracted from lignocellulosic biomass, emerges as a beacon of hope for conversion into value-added chemicals. However, the inherent susceptibility of its unsaturated aldehyde groups to excessive oxidation often culminates in undesired reactions, compromising both the yield and specificity of the desired products.
View Article and Find Full Text PDFHeterotrophic nitrification, similar to autotrophic nitrification, involves key enzymes and reactive nitrogen intermediates during ammonia oxidation, which may influence antibiotic transformation. However, the interference between antibiotic transformation products from ammonia oxidation and secondary metabolites in heterotrophic nitrifiers makes antibiotic transformation pathways more complicated. In this work, we observe that the heterotrophic nitrifier Alcaligenes ammonioxydans HO-1 can effectively convert sulfonamide antibiotics.
View Article and Find Full Text PDFWastewater surveillance programs based at wastewater treatment plants (WWTPs) have been widely implemented, becoming a crucial measure for public health. Recently, the scope of monitoring has expanded from influent wastewater to include primary settled solids and activated sludge. The effectiveness of monitoring primary settled solids has been widely validated, but the suitability of activated sludge as a monitoring target remains unclear.
View Article and Find Full Text PDFOrganic pollutants removal via a polymerization transfer (PT) pathway based on the use of single-atom catalysts (SACs) promises efficient water purification with minimal energy/chemical inputs. However, the precise engineering of such catalytic systems toward PT decontamination is still challenging, and the conventional SACs are plagued by low structural stability of carbon material support. Here, we adopted magnesium oxide (MgO) as a structurally stable alternative for loading single copper (Cu) atoms to drive peroxymonosulfate-based Fenton-like reactions.
View Article and Find Full Text PDFUranium is the primary fuel for nuclear energy, critical for sustainable, carbon-neutral energy transitions. However, limited terrestrial resources and environmental risks from uranium contamination require innovative immobilization and recovery solutions. In this work, we present a novel uranium recovery method using programmable electroactive living materials (ELMs).
View Article and Find Full Text PDFIron (hydro)oxides are commonly used to enhance anaerobic digestion due to their cost-effectiveness and versatility. However, the influence of crystalline structure on digestion performance is often overlooked despite their unique characteristics. In this study, we investigated how different crystalline forms of FeOOH affect substrate utilization, sludge activity, and the microbiomes in up-flow anaerobic sludge blanket (UASB) reactors.
View Article and Find Full Text PDFFlow-electrode capacitive deionization (FCDI) is a promising electrically driven technology for brackish water desalination, but it suffers from scaling issues in the concentrate chamber when treating brackish water with high levels of SO and Ca. In addition, how the key components (e.g.
View Article and Find Full Text PDFResearch (Wash D C)
November 2024
Activating the ultralong room-temperature phosphorescence (RTP) of mono-ring arylboronic acid remains a great challenge, because the capacious free spaces shaped by a rubbery polymeric matrix allow the benzene ring skeleton to freely rotate. Herein, the ultralong RTP in mono-ring arylboronic acid derivatives embedded in a polyvinyl alcohol (PVA) matrix is activated, leveraging enhanced intermolecular and intramolecular hydrogen bonding and activating ultralong RTP. By incorporating diverse PBA derivatives into PVA via click chemistry, 3-aminophenylboronic acid (3A-PBA) doped PVA films showcase the most extended RTP lifetimes (2.
View Article and Find Full Text PDFExploiting electrogenic microorganisms as unconventional chassis hosts offers potential solutions to global energy and environmental challenges. However, their limited electrogenic efficiency and metabolic versatility, due to genetic and metabolic constraints, hinder broader applications. Herein, we developed a multifaceted approach to fabricate an enhanced electrogenic chassis, starting with streamlining the genome by removing extrachromosomal genetic material.
View Article and Find Full Text PDFFungal laccase producers can effectively address bisphenol A (BPA) and antibiotic-contaminated water. However, the role of small mediators produced by fungal secondary metabolism in enhancing the removal of refractory contaminants is often overlooked. In this work, an efficient laccase-producing strain, Trametes hirsuta La-7, was activated to simultaneously treat BPA and antibiotics.
View Article and Find Full Text PDFThe operation of membrane-based reactors is inevitably challenged by fouling. The driving force in these reactors is not only critical for water passage through membranes but also significantly influences fouling, such as biocake formation. This study investigated the differences between biocakes formed under transmembrane pressure (TMP) and forward osmosis (FO) conditions, specifically focusing on their components, spatial structures, and microbial communities.
View Article and Find Full Text PDFEnviron Sci Technol
October 2024
Advanced oxidation processes (AOPs) are rapidly evolving but still lack well-established protocols for reliably identifying oxidative reactive species (ORSs). This Perspective presents both the radical and nonradical ORSs that have been identified or proposed, along with the extensive controversies surrounding oxidative mechanisms. Conventional identification tools, such as quenchers, probes, and spin trappers, might be inadequate for the analytical demands of systems in which multiple ORSs coexist, often yielding misleading results.
View Article and Find Full Text PDFNitrogen compounds in current seawater treatment processes typically are converted to nitrate, threatening seawater quality and marine ecology. Electrochemical denitrification is a promising technique, but its efficiency is severely limited by the presence of excess chloride ions. In this work, a flow-through cell went through an on-demand chlorine-mediated electrochemical-chemical tandem reaction process was designed for efficient seawater denitrification.
View Article and Find Full Text PDFThe artificial photocatalytic synthesis based on graphitic carbon nitride (g-CN) for HO production is evolving rapidly. However, the simultaneous production of high-value products at electron and hole sites remains a great challenge. Here, we use transformable potassium iodide to obtain semi-crystalline g-CN integrated with the I/I redox shuttle mediators for efficient generation of HO and benzaldehyde.
View Article and Find Full Text PDFWhile flow-electrode capacitive deionization (FCDI) is recognized as an attractive desalination technology, its practical implementation has been hindered by the ease of scaling and energy-intensive nature of the single-cell FCDI system, particularly when treating brackish water with elevated levels of naturally coexisting SO and Ca. To overcome these obstacles, we propose and design an innovative ion-selective metathesis FCDI (ISM-FCDI) system, consisting of a two-stage tailored cell design. Results indicate that the specific energy consumption per unit volume of water for the ISM-FCDI is lower (by up to ∼50%) than that of a conventional single-stage FCDI due to the parallel circuit structure of the ISM-FCDI.
View Article and Find Full Text PDFDeveloping eco-friendly catalysts for effective water purification with minimal oxidant use is imperative. Herein, we present a metal-free and nitrogen/fluorine dual-site catalyst, enhancing the selectivity and utilization of singlet oxygen (O) for water decontamination. Advanced theoretical simulations reveal that synergistic fluorine-nitrogen interactions modulate electron distribution and polarization, creating asymmetric surface electron configurations and electron-deficient nitrogen vacancies.
View Article and Find Full Text PDFThe development of in situ techniques to quantitatively characterize the heterogeneous reactions is essential for understanding physicochemical processes in aqueous phase. In this work, a new approach coupling in situ UV-vis spectroscopy with a two-step algorithm strategy is developed to quantitatively monitor heterogeneous reactions in a compact closed-loop incorporation. The algorithm involves the inverse adding-doubling method for light scattering correction and the multivariate curve resolution-alternating least squares (MCR-ALS) method for spectral deconvolution.
View Article and Find Full Text PDFAppropriate mixed carbon sources have great potential to enhance denitrification efficiency and reduce operational costs in municipal wastewater treatment plants (WWTPs). However, traditional methods struggle to efficiently select the optimal mixture due to the variety of compositions. Herein, we developed a machine learning-assisted high-throughput method enabling WWTPs to rapidly identify and optimize mixed carbon sources.
View Article and Find Full Text PDFJ Colloid Interface Sci
October 2024
Artificial photosynthesis using carbon nitride (g-CN) holds a great promise for sustainable and cost-effective HO production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I/I) intercalation through a pre-photo-oxidation process using potassium iodide (suspected deteriorated "KI") within the g-CN framework. Moreover, we introduce an external electric field by incorporating cationic methyl viologen ions to establish an auxiliary electron transfer channel.
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