Latest ArticlesNitrate contamination has prompted global concern due to its far-reaching effects on human health and the ecosystem. As an emerging technology, electrochemical nitrate reduction reaction (eNO3RR) provides a promising approach for converting nitrate to valuable ammonia (NH3) or harmless nitrogen gas (N2). However, the conversion efficiency of eNO3RR is still constrained by the mismatch between catalysts and the reaction microenvironment at lower nitrate concentrations (< 0.1 mol/L). In this review, we have systematically discussed the feasibility of electrochemical methods in treating low-concentration nitrate by summarizing recent advances and their reaction mechanisms. Meanwhile, the selection between NH3 and N2 pathways was evaluated based on the nitrate concentration range and safety considerations associated with each scenario. Finally, the dominant factors for applying eNO3RR to real-world scenarios were also thoroughly discussed. We hope this review can provide comprehensive insights into the design of optimal catalysts and systems for treating low-concentration nitrates in practical scenarios, thereby promoting the environmental sustainability of electrocatalytic technologies.
Catalytic oxidation of H2S at room temperature has been regarded as a promising method for removing malodorous H2S pollution. However, most of the existing research has primarily focused on developing catalysts with high sulfur capacity, i.e., high elemental sulfur selectivity, which was unfavored for the catalyst regeneration. The present work prioritizes efficient water wash regeneration as a key objective. A series of activated carbon fibers (ACFs) was synthesized using a synergistic strategy of "nitrogen doping-plasma defect engineering". The certain amount of nitrogen species ensured a certain level of sulfur capacity. The plasma defect engineering can result in the enhancement of surface acidity and defect density, which worked together to make the catalyst with high sulfate selectivity. The O2-plasma modified NH3-ACF-O10 catalyst achieved the best catalytic performance with appropriate sulfur capacity (0.21 g/g) and highest sulfate selectivity (85.40%). Importantly, it can be easily regenerated by water wash, and almost 83.33% sulfur capacity can be recovered. Besides, superoxide radicals (O2•-) were identified as the primary reactive oxygen species for the reaction. And the reaction obeyed a Langmuir-Hinshelwood (L-H) like mechanism, i.e., the reaction was proceeded via chemisorbed H2S and O2•-, which was adsorbed and activated by defect.
Rare–earth–based perovskite materials, due to their low cost and tunable structure, have been regarded as a promising platform for photoinduced molecular oxygen activation. However, a comprehensive understanding and precise regulation of the surface reconstruction of the active phase in perovskite oxides during molecular oxygen activation remain highly challenging tasks. Herein, a refined A–site management strategy is proposed for perovskite oxides, which provides power for molecular oxygen activation by adjusting the electronic structure of B–site elements. Comprehensive experimental results reveal that the enhanced photocatalytic mechanism is attributed to the substitution of holmium (Ho) at the atomic level, which facilitates an increase in the valence state of iron and shifts the center of the d–band to a more positive energy level, thereby promoting O2 adsorption. Additionally, theoretical calculations demonstrate that the Ho 4f orbital overlaps with the Fe 3d and O 2p orbitals near the Fermi level, significantly enhancing charge transfer between oxygen and metal, thereby facilitating the conversion of oxygen into highly reactive oxygen species. Therefore, the optimized La0.97Ho0.03FeO3 (LHFO) exhibits greatly enhanced catalytic performance for molecular oxygen activation, and the degradation rate constant of tetracycline is 9.5 times higher than LaFeO3, representing one of the most efficient and robust RE–based perovskites.
Achieving point-of-care detection of neutrophil gelatinase-associated lipocalin (NGAL) contributes to the early diagnosis and treatment of acute kidney injury (AKI), but the lack of highly sensitive and long-term stable detection methods is a major challenge. In this work, tetrahedral DNA (tDNA)-functionalized large-sized upconversion nanoparticles (t-UCNP300) were synthesized with high luminescence intensity. Leveraging the dual effects of surface charge density and the rigid structure of tDNA, the developed t-UCNP300 exhibited long-term stability for over 60 days after being stored in phosphate buffer at 25 ℃ and pH 7.4, with no obvious aggregation and only slight luminescence attenuation. By using this developed t-UCNP300, a luminescent lateral flow immunoassay (LFIA) strip was developed for point-of-care detection of NGAL, with a detection linearity range of 2.00–250 ng/mL and limit of detection (LOD) of 1.00 ± 0.07 ng/mL (S/N = 3). Taking advantage of the developed LFIA strip for NGAL with high selectivity and a rapid response time of < 5 min, it was successfully applied for the determination of NGAL in artificial urine samples.
The wastewater produced in the antibiotic manufacturing process is a significant source of antibiotic pollution in the aquatic environment, posing a severe threat to ecological health and human well-being. Researchers have explored various methods, including source reduction technologies such as enzymatic engineering and green process control, to enhance antibiotic extraction efficiency. In addition, high-efficiency end-of-line processing technology has also been widely developed. This review first provides a detailed introduction to the characteristics of various antibiotics and their distribution levels in the environment. Then we systematically summarize and analyze the full-chain antibiotic end-of-pipe treatment processes, including conventional treatment processes and typical advanced treatment processes. Especially compares and analyzes the removal efficiency and carbon emissions of different conventional treatment processes, aiming to select efficient and low-carbon treatment processes. We intend to provide effective solutions to tackle the issue of antibiotic pollution while ensuring public health and ecological security.
Understanding the nucleation, growth and structural phase transitions process during the preparation of nanomaterials is crucial for the targeted design and controllable preparation of nanomaterials with specific structures and properties. Herein, a “solid phase transition” behavior is first found in the semiconductor C3N4 material during the conversion process from amorphous bulk C3N4 to high crystallinity C3N4 nanosheets, which usually exists in the process of metals or alloys conversion. A unique C3N4 nanosheet structure with uniform size distribution is successfully synthesized with a simple two-step calcination method, which is totally different from the traditional irregular nanosheets exfoliated from the bulk C3N4. This C3N4 nanosheets also possess high crystallinity and it helps to promote the migration of charge carriers during the catalytic process. By precisely exploring the synthesis process, a new “solid phase transition” mechanism is introduced to help understand the atoms recrystallize and grow to form the uniform high crystallinity nanosheets. The high yield (86%) of this strategy also overcomes the problem of low efficiency in preparing C3N4 nanosheets. Besides, the advantages of this uniform high crystallinity C3N4 nanosheets result in superior long-term stability in 100 CV cycles during the electrochemiluminescence (ECL) test, which is particularly superior to conventional C3N4 nanosheets.
Electroactive quinone-based compounds have shown great potential as lithium-ion batteries cathodes due to their high capacity, environmental friendliness, and low cost. However, their practical application is severely hindered by high solubility in aprotic electrolytes and low electronic conductivity. Herein, we skillfully utilized the two-dimensional MXene Ti2C2 as a host material to anchor benzoquinone skeleton by a simple coordination chemical reaction, obtaining the composite cathode materials (T@M). Significantly, the MXene not only stabilizes the benzoquinone framework but also shortens ion/electron diffusion pathways. As a result, the T@M cathode delivers a high discharge specific capacity of 300.1 mAh/g at 0.05 A/g and retains 70% of its capacity after 3000 cycles at 1 A/g. This work provides an effective strategy for developing high-performance organic electrodes for rechargeable batteries.
As a new wastewater treatment technology, the microalgae-fungi consortia system (MFCS) has attracted much attention because of its high efficiency, environmental protection and energy saving features. Extracellular polymeric substances (EPS) play a key role in MFCS treatment of wastewater and microalgae harvesting. In this review, the definition and formation process of MFCS, thoroughly examines the composition, properties, and influencing factors of EPS, as well as systematically explains the mechanism of action of EPS in wastewater treatment and microalgae harvesting. EPS surface functional groups have negative charge, adsorption, flocculation, and hydrophilicity/hydrophobicity properties. Microalgae and fungi form MFCS through EPS electrostatic attraction and protein bridging. EPS achieves adsorption, aggregation, and degradation of pollutants through targeted binding, chelation, coordination mechanisms, hydrophobic interactions, and complexation degradation mechanisms via functional groups. EPS achieves microalgae harvesting through electrostatic neutralization, surface protein interaction, and polysaccharide adhesion. However, current research still faces the following challenges, the selection of algal strains in the formation process of MFCS is still unclear. The mechanism of EPS removal of new pollutants and internal signaling pathways are still unclear. FSH takes too long, while FPH requires higher costs during harvesting. In the future, MFCS should be explored in combination with actual engineering applications, and different combinations of algae species and strains should be explored. Using genetic engineering to explore the synergistic mechanism of microalgae and fungi EPS in pollutant treatment. Improve the process conditions for harvesting microalgae using fungi, optimizing the two methods of microalgae harvesting, and conduct experiments on the efficient harvesting of microalgae. This review systematically explored the mechanism of action of EPS in MFCS, which is important for wastewater treatment and microalgal biomass harvesting.
Marine atmospheric aerosols are pivotal components of the global aerosol system, which can significantly influence global climate and human health. Perfluoroalkyl carboxylic acids (PFCAs), persistent emerging contaminants, exhibit pronounced enrichment in sea spray aerosols (SSAs). However, current gas-particle partitioning models underestimate their particulate-phase ratios in polluted atmospheres. Here, we elucidate the interfacial chemistry driving the enrichment of PFCAs in SSAs under anthropogenic impacts. Through Born-Oppenheimer molecular dynamics simulations, we demonstrated that TFA, a representative of PFCAs, exhibited activity at gas-liquid interfaces. The carbonyl oxygen of TFA protrudes beyond hydration layers, which facilitates collisions with gaseous SO3. Interfacial water molecules can promote simultaneous TFA deprotonation and SO3 collision and then the formation of trifluoroacetic acid sulfuric anhydride ions (TFASA-) and hydronium ions (H3O+). TFASA- displays superior hygroscopicity over precursors, enhancing the growth potential of SSAs to form cloud condensation nuclei (CCN). Given the continuous accumulation of PFCAs in marine environment, the interfacial chemical reactions between PFCAs and reactive pollutants (e.g., SO3) in marine atmospheres need urgent focus to understand the influence of PFCAs on marine particulate matter pollution and global climate.
In heterogeneous Fenton-like systems, the oxidative polymerization pathway is of great significance in the field of sustainable water treatment. Unlike the traditional mineralization pathway, it can convert organic pollutants into polymers, thereby achieving the recovery of carbon resources. This paper focuses on the core content related to this pathway, expounding that the mechanism of oxidative polymerization is influenced by multiple factors (catalysts, oxidants, organic matters). Meanwhile, various methods exist for identifying the polymerization pathway, such as electrochemical experiments, Raman spectroscopy analysis, and mass spectrometry technology, which can infer the reaction process and product structure. Additionally, this paper reveals two pathways for pollutant removal through oxidative polymerization: The radical pathway and the non-radical pathway. In the future, advanced characterization techniques should be used to deeply explore the microscopic mechanism of oxidative polymerization, optimize catalyst design, expand practical application research, and explore comprehensive utilization pathways for its products, so as to promote the development of sustainable water treatment technologies.
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