JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
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MEASUREMENT
·
2025
·
IF 5.6
Jintao Liang,Zhenshun Wei,Qing Huang,Jianlu Liang,XiuChuan Zhao,Zhide Zhou,Guiyin Li
Tea polyphenols are a general term for the total phenolic compounds in tea. Tea polyphenols play a crucial role in the quality of tea. Rapid detection of tea polyphenols is essential for tea harvesting and breeding. In this paper, a rapid method for the detection of tea polyphenols is presented based on diazotization coupling (DC) reaction and flow batch analysis system (FBAS). The tea polyphenols detection based on DC reaction can avoid interference from non-phenolic substances and improve detection accuracy. Meanwhile, FBAS for sample injection can shorten the analysis time, reduce the reagent consumption and improve the sensitivity. Experimental results demonstrate that absorbance values exhibit linearity with gallic acid concentrations in the range of 5 to 60 μg/mL, with a linear equation of y = 0.0279x + 0.0613 (R 2 = 0.9993) and a limit of detection (LOD) of 0.215 μg/mL (S/N=3). The method was applied to the detection of tea polyphenols in tea samples, with relative standard deviations (RSD) ranging from 0.326% to 0.659%. The DC-FBAS method has a high potential application with the requirements of portable, cost-effective, and highly precise on-site tea polyphenols detection.
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Materials Chemistry Frontiers
·
2025
·
IF 6.4
Lijie Qi,Yu Fu,borui ji,Bauyrzhan Sarsenbekuky,Wanli Kang,Hongbin Yang,Shujun Liu
Electrochemical synthesis of ammonia (NH₃) through cathodic nitrate reduction presents an effective alternative to the Haber-Bosch process, enabling efficient ammonia production without significant environmental pollution. Electrocatalytic degradation strategy is an efficient and environmentally friendly tool for the treatment of oily wastewater containing partially hydrolized polyacrylamide (HPAM). Thus, coupling cathodic nitrate reduction with anodic HPAM oxidation can further enhance ammonia synthesis efficiency and HPAM degradation efficiency. Here, we reported an N-doped carbon nanotube loaded with CuNi-x (X = 0.5, 1, 2) as an electrocatalyst for cathodic nitrate reduction coupled with anodic HPAM oxidative degradation. Notably, the CuNi-1 variant achieved the highest ammonia yield of 4962.76 ± 40.22 μg h-1 mgcat-1 and a Faradaic efficiency of 85.91 ± 0.42%. Furthermore, the oxidative degradation rate of HPAM reached a maximum of 81.91 ± 0.36% within 2 h. Anodic HPAM oxidation not only promotes cathodic nitrate reduction but also enables the acquisition of valuable anodic products. Using in-situ ATR-SEIRAS, in-situ DEMS, and DFT calculations, we thoroughly analyzed reaction intermediates and the critical role of the CuNi bimetallic system in electrocatalytic nitrate reduction. The coupled reaction system was established to achieve both efficient ammonia synthesis and HPAM degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhimo Fang,Yuan Liang,Zepeng Zeng,Haotian Bai,Zhou Zhou,Lin Zhang,Bin Hu,Shiguan Yang,Jihong Li,Qiang Lu
Herein, we synthesized well-dispersed N and Fe-doped CoS 2 (FNCS) with stable sulfur vacancies (S V ) for Fenton-like reaction. The characterization, experimental, and calculation results jointly unveiled the synergistic modification of heteroatoms and defects within FNCS constructed unique Co−N−Fe···S V sites, enabling synchronous activation of peroxymonosulfate (PMS) and dissolved oxygen (DO). Optimized S 3p-Co 3d orbital hybridization facilitated efficient electron cycling, generating both SO 4 •− radicals and singlet oxygen ( 1 O 2 ) at Co−N−Fe···S V sites. Consequently, the FNCS/PMS system, operating via a radical-nonradical synergistic mechanism, achieved an ultra-high pollutant degradation rate constant of 2.71 min⁻¹ , 3.77 times higher than radical-dominated CoS 2 /PMS, while retaining over 90 % of its initial activity after 10 h of operation with strong interference resistance. This work provides a clear perspective on regulating the electronic structure of active sites to synergistically activate multiple oxidants for enhanced Fenton-like catalysis.
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ChemistrySelect
·
2024
·Vol. 9
·期 10
·e202303652
·
IF 1.9
Huanhuan Ma,Na Zhang,Xinzhu Wang,Kui Lin,Ping Liu,Fei Tian
Graphical A green one-step hydrothermal method has been successfully used to prepare carbon dots (CDs) by selectively co-doping nitrogen, phosphorus and sulphur elements. For the sensitive detection of iron ions, a fluorescence quencher sensor based on nitrogen- and sulphur-doped carbon dots (red NS-CDs) has been developed, because of the good optical properties and bio-histocompatibility of green NPS-CDs and blue NP-CDs, They are observed to penetrate NCl−H292 cells, fluorescing green and localizing in the cytoplasm. Carbon dots (CDs) with tunable photoluminescence was successfully prepared via selective co-doping of three elements, including nitrogen, phosphorus and sulfur element by green one-step hydrothermal method. Nitrogen-sulfur-doped CDs (red NS-CDs), which emitted red fluorescence under UV excitation, were used to detect iron ions in the linear range 1–50 μM, yielding detectable limits as low as 94 nM. The nitrogen-phosphorus-doped CDs (blue NP-CDs) exhibited blue fluorescence with quantum yields up to 34.5 %. When the concentration is 800 μg/mL, it showed excellent anticancer effect in vitro. The nitrogen-sulfur-phosphorus-doped CDs (green NPS-CDs) emitting green fluorescence showed a low cytotoxicity at a high concentration of 800 μg/mL and were used for intracelluar imaging of NCl−H292 cells. This study demonstrated the photoluminescent characteristics of carbon dots (CDs) and highlighted the ability to modify their peak fluorescence emission wavelengths through the flexible combination of specific reagents under comparable hydrothermal conditions. Additionally, it provided valuable insights into the efficient methodologies for synthesizing CDs suitable for various application scenarios.
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Molecular Catalysis
·
2025
·
IF 4.9
Binxin Lv,Jiayue Yu,Fengchen Zhou,Zizi Wang,Junjun Zhang,Yifan Zhang,Yang Wu,Yong Wang,Wen Luo
Urea electrosynthesis plays a vital role in the nitrogen cycle, promoting carbon neutrality while also being energy-efficient. However, the complexities involved in the simultaneous of carbon and nitrogen-containing species significantly hinder the selectivity and yield of urea. In this study, we report a CuZn bimetallic catalyst that is capable of converting CO 2 and NO 3 ⁻ into urea, with a maximum Faraday efficiency of 40% at -0.6 V vs. RHE, alongside an impressive urea yield rate of 304.8 mmol h ⁻¹ g cat ⁻¹ at -0.9 V vs. RHE, surpassing the performance of both monometallic Cu and Zn catalysts. In situ spectroscopic analysis demonstrates that the Cu sites within CuZn facilitates the adsorption and activation of CO 2 and NO 3 ⁻ , while Zn sites additionally facilitate CO 2 adsorption and reduces the adsorption strength of *CO and *NH 2 on the catalyst surface, collectively promoting the formation of *CONH 2 as a key intermediate in urea synthesis. This study highlights the unique role of zinc in urea synthesis, offers new insights into optimizing the performance of copper-zinc catalysts, and serves as a valuable reference for future research on the role of zinc in urea synthesis.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2025
·
IF 6.1
Weishou Shen,Yang Wu,Futao Li,Shirui Zhang,Hongmei Jin,Bei Gao
Microplastics, as emerging contaminants, can absorb antibiotics, and their coexistence in soil ecosystems poses serious threats to soil health. While previous studies have primarily focused on the individual effects of microplastics or antibiotics, the interactions between these pollutants in soil environments remain poorly understood. In this study, we investigated the combined effects of sulfonamide antibiotics and microplastics—both non-degradable low-density polyethylene and degradable polylactic acid—on soil microbiota and physicochemical properties. Our findings revealed significant changes in soil properties under co-exposure conditions. Dissolved organic carbon emerged as the most influential factor affecting bacterial and fungal diversity. Co-exposure altered the composition of bacterial and fungal communities at both the phylum and genus levels, with soil bacteria showing stronger responses than fungi. Importantly, co-exposure exacerbated the ecological risks associated with individual contaminants. We also observed differences in how non-degradable and degradable microplastics impacted the stability and complexity of microbial community networks. Notably, co-exposure to degradable microplastics and sulfonamides led to a significant increase in the expression of antibiotic resistance genes ( sul1 and int1 ). These findings enhance our understanding of the combined effects of microplastics and antibiotics on soil ecosystems and underscore the need for further research into their ecological risks.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Junjie Chen,Xiaomei Xing,Sisi Wen,Mengyuan Li,Di Liu,Wenji Jiang,Xinyi Shao,Ruikai Qi,Yumei Yang,Ming Mu,Zheng-jie Chen,Bing Zhao,Wei Song
The pursuit of efficient ammonia production through electrochemical nitrate reduction reaction (NO 3 RR) at ambient conditions is a significant demand in green and energy-saving industries. Rational tailoring of the competing yet complementary processes of water splitting and nitrate activation at reducing potentials is pivotal for manipulating the efficiency and selectivity of ammonia synthesis. Herein, Ag 92 Ru 8 aerogel has been synthesized via a one-step reduction strategy, demonstrating remarkable in tuning the reaction intermediates and interfacial water dynamics. Based on Ag 92 Ru 8 aerogels, a high NH 3 Faradaic efficiency (FE) of 97.16 %, and a superior yield rate of 2.49 mmol h −1 mg cat. −1 were achieved at −0.5 V . And the corresponding Zn-NO 3 − battery exhibited potential as a power source for practical application. In-situ surface-enhanced Raman spectroscopy (SERS) and density functional theory (DFT) results demonstrate that H* intermediate generated from interfacial water are promoted by Ru species in the hydrogenation process of NO 3 RR, offering valuable insights for the targeted design of efficient catalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Yu Lei,Chen Cheng,Yangjian Zhou,Xiaoran Chen,Xin Lei,Wenjing Song,Zhimin Qiang,Chuncheng Chen,Jincai Zhao
More frequent global wildfire events intensify the exposure risks of nitrophenols through brown carbon (BrC) emissions. Radical reactions dominate the fates of nitrophenols in surface, municipal, and atmospheric waters, yet the involved reaction kinetics and mechanisms remain poorly understood. In this work, by combining transient and steady-state multispectral analyses, the second-order rate constants (k) for nitrophenols and biomass-burning BrC reacting with HO• as well as common secondary radicals (e.g., Cl2•–, CO3•–, and NO3•) were determined (k ≈ 105–1010 M–1 s–1 at pH 2.0–10.0 for both protonated and deprotonated nitrophenols), most of which are reported for the first time. We also experimentally demonstrated that the reactions of nitrophenols and BrC with various radicals could produce a substantial amount of HONO/NO2– (a key precursor of tropospheric HO•), with molar yields reaching ∼50%. Mechanistic investigations revealed that the phenoxy radical (PhO•), generated from either single electron transfer or addition–elimination reactions during the radical reactions of nitrophenols, acted as a universal intermediate for the denitration. Hence, the new kinetic and mechanistic insights suggest that the radical-induced denitration process of BrC and nitrophenols in acidic waters may serve as a previously overlooked HONO source, but such denitration does not guarantee detoxification due to the simultaneous generation of high-risk biphenols. This work highlights the critical role of secondary radicals in nitrophenols and BrC transformation across different waters, shedding light on several unforeseen chemical impacts driven by intensified global wildfires.
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CURRENT MICROBIOLOGY
·
2025
·Vol. 82
·期 9
·1-11
·
IF 2.6
Gu Yiwen,Lin Xiu,Lu Yanxu,Fang Shuguang,Hu Kun,Ju Xin,Li Liangzhi,Chen Zhi
The increasing use of antibiotics in shrimp aquaculture has raised concerns regarding ecological safety and the emergence of antibiotic resistance. This study aimed to isolate and characterize probiotic lactic acid bacteria (LAB) strains from the gut of Penaeus vannamei to evaluate their potential as antibiotic alternatives in aquaculture. Two strains, S1 and S2, were identified with 99.79 and 99.51% similarity to Pediococcus acidilactici DSM 20284 and Enterococcus lactis BT159, respectively. Based on minimum inhibitory concentration (MIC) assays, both strains exhibited high sensitivity to the tested antibiotics. They also demonstrated notable acid and bile salt tolerance, with S1 maintaining a survival rate of 30% at pH 5 and S2 achieving 40% survival at pH 6. Under 0.03% bile salt concentration, survival rates were approximately 60% (S1) and 45% (S2), while S1 retained 15% viability even at 0.9% bile salt. Enzymatic activity analysis indicated that both strains exhibited lower amylase activity compared to other hydrolytic enzymes, with S2 showing higher cellulase and protease activities than S1. Antimicrobial assays revealed that both strains exerted broad-spectrum inhibition against four indicator pathogens. S1 exhibited the strongest inhibitory effect against Aeromonas hydrophila (inhibition zone: 1.6–2.2 cm), whereas S2 showed the highest inhibition against Vibrio parahaemolyticus (1.5–2.4 cm). Feeding trials demonstrated that the combined application of S1 and S2 significantly enhanced shrimp body weight (6.05 ± 0.09 g vs. 9.23 ± 0.2 g, P < 0.01) and survival rate (62.49% ± 1.56 vs. 93.78% ± 2.55, P < 0.01). These findings highlight the potential of Lactobacillus strains as probiotics in shrimp farming, offering a sustainable approach to reducing antibiotic dependency and improving shrimp health and productivity.
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ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2025
·Vol. 47
·期 8
·1-20
·
IF 3.8
Hu Zhengchun,Huang Xinrui,Shen Wu,Guo Minghao,Liao Bing
Leakage and migration of landfill leachate are often accompanied by complex biogeochemical processes that form a continuous series of redox zones in the leachate plume. Nitrogen in leachate, especially NH 4 ⁺-N, is one of the most important pollutants contributing to groundwater contamination. While traditional landfill pollution prevention and control measures often have difficulty effectively addressing the complex migration and transformation behaviors of NH 4 ⁺-N in leachate, an in-depth study of the migration and transformation processes of NH 4 ⁺-N in the redox compartment is crucial for the development of accurate and efficient pollution prevention and control strategies. In this study, static transformation experiments, dynamic simulated column experiments and high-throughput sequencing techniques were used to systematically investigate the migration and transformation processes of NH₄⁺-N in the redox bands of a simulated landfill. The results showed that in the NH 4 ⁺-N transformation experiment, the soil in the simulated oxidation zone had the strongest ability to transform NH 4 ⁺-N, with the NH 4 ⁺-N concentration decreasing from 40 to 0.03 mg/L, whereas the sterilization treatment completely suppressed the transformation process of NH 4 ⁺-N in the OZ. The NH 4 ⁺-N in the continuous redox zone completely penetrated the simulated soil column on the 7th day, and the maximum effluent concentration was stable in the range of 1530 ± 30 mg/L. The trends of NH 4 ⁺-N in each independent redox zone were consistent, with the TZ having the richest microbial community abundance and number of species, and some Acidobacteria were able to reduce Fe(III) under anoxic conditions and interact with the organic matter, which effectively contributed to the cycling of Fe within the TZ. These findings indicate that there are significant differences in the biogeochemical cycling process of NH 4 ⁺-N in different redox zone environments, and this study provides a new research perspective for a deeper understanding of the biogeochemical cycling mechanism of the elements in landfills and an important scientific basis for the prevention, control, and remediation of landfill pollution.
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ACS Nano
·
2025
·
IF 16
Lixin Xu,Shumin Chen,Baipeng Yin,Hao Jia,Jinjie Hao,Qingda Chang,Yu Zhang,Chuang Zhang,Jiannian Yao
Electrochemical deposition is a facile and effective method for the in situ growth of metal electrocatalysts; however, it is difficult to optimize their morphology and performance due to the kinetics-controlled growth at high current density. Herein, we develop a new magneto-electrochemical deposition technique to prepare the faceted microcrystals of copper (Cu) catalysts for highly efficient electrocatalytic nitrate-to-ammonia conversion. The field generates a Lorentz force on the flow of Cu ions near the cathode surface, which retards the mass transport to predeposited Cu particles and increases the density of Cu nucleation sites due to the magnetohydrodynamics (MHD) effect. This further slows down the growth rates of individual Cu particles at even high current density, and as-prepared Cu catalysts change from low-crystalline microspheres to thermodynamic-controlled faceted microcrystals. Especially, these Cu microcrystals show a very high exposure of (111) facet, which provides an energy-efficient reaction pathway for nitrate reduction. The magneto-electrochemically deposited Cu microcrystals exhibit a high Faradaic efficiency of >95% for nitrate-to-ammonia conversion with an excellent stability over 60 h, which indicates that the magneto-electrochemical deposition provides a promising way to the design and synthesis of high-quality electrocatalysts for advanced catalytic applications.
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