JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Lisong Xia,Lei Cheng,Wenni Xi,Xiliang Zhang,Xianyang Shi
The environmental fate and risks of mononitrophenols (mono-NPs), the simplest nitrophenols (NPs) often found in aquatic environments, are profoundly influenced by anaerobic bioreduction and co-existing electron shuttles (ESs), but little is known about the underlying mechanisms. Here, we elucidate the pathways of anaerobic mono-NPs bioreduction by Shewanella oneidensis MR-1 and assess the effect of model ESs on these processes. We found that all three mono-NPs isomers could be readily reduced to their corresponding aminophenols by S. oneidensis MR-1 under anaerobic conditions. CymA, a core component of the Mtr respiratory pathway, performs a dynamic role in these bioreduction, which is highly dependent on the bioreduction kinetics. The exogenous addition of quinones was found to accelerate the mono-NPs bioreduction through interactions with key outer-membrane proteins (e.g., OmcA and MtrC), and all these processes matched well to linear free energy relationships (LFERs). Surprisingly, adding riboflavin did not influence the bioreduction of all three mono-NPs isomers, which may be due to the contribution of OmcA and MtrC to these bioreduction processes and their downregulated expression. This study enhances our understanding of the environmental fate of mono-NPs and their bioconversion processes, providing valuable insights for the bioremediation of nitrophenol-contaminated sites.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Hong Chen,Peng Wu,Lu-Bin Zhong,Qi-Jun Zhang,Mohammad Younas,Yu-Ming Zheng
Rapid industrialization and urbanization have significantly increased wastewater discharge into natural water bodies, thereby emphasizing the critical importance of precise long-term pollutant monitoring at urban sewage outfalls to protect aquatic ecosystems. Free chlorine (FC), widely used in disinfection, poses significant ecological risks when overdischarged. However, achieving reliable long-term FC monitoring at discharge points remains a substantial challenge. In this study, we developed a continuously responsive surface-enhanced Raman scattering (SERS) sensor for long-term on-site FC monitoring. The sensor integrated a flexible SERS probe functionalized with 4-aminothiophenol (4-ATP) for selective FC detection and a compact floating roller device for continuous signal acquisition. The sensor exhibited a low detection limit of 4.16 ppb and accurately quantified FC concentrations in real-world water samples, showcasing high sensitivity and reliability. Long-term deployment at sewage treatment plant (STP) outfalls further validated its robust monitoring capabilities under actual environmental conditions. This innovative SERS sensor offers a practical and accurate solution for long-term on-site FC monitoring, highlighting its potential as a scalable approach for environmental monitoring applications.
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Environmental Chemistry and Ecotoxicology
·
2025
·
IF 8.2
Yanhua Wang,Zhengli Tang,Yingnan Liu,Yilin Qian,Shuo Yang,Anqi Wang,Zhibao Dong,Baoshan Xing
Microplastics (MPs) aggregation critically governs their environmental transport, yet interactions with mineral surfaces remain underexplored. In this study, polyethylene (PE) MPs were employed as model particles to prepare both pristine PE and bovine serum albumin (BSA)-coated PE (B-PE). The heterogeneous aggregation of these particles with inorganic minerals (goethite, hematite, pyrite, magnetite) and clay minerals (kaolinite, montmorillonite) was systematically investigated under varying pH conditions (3.0, 6.0, 9.0) and ionic strengths (NaCl 5–300 mmol/L, CaCl 2 1–50 mmol/L). Results demonstrated that positively charged inorganic minerals exhibited significantly stronger heterogeneous aggregation with negatively charged PE, exhibiting aggregation capacities 2.97 times higher than those of negatively charged clay minerals. The introduction of oxygen-containing functional groups such as COOH and OH on the B-PE surface not only enhanced electrostatic attraction but also facilitated ligand exchange and hydrogen bonding, further improving aggregation efficiency. At pH 3.0, removal efficiencies of PE and B-PE for inorganic minerals exceeded 90 %, while aggregation was nearly completely inhibited at pH 9.0. With increasing NaCl concentration, the critical coagulation concentration (CCC) of B-PE decreased by 29.6 %–42.6 % compared to pristine PE. Moreover, Ca 2+ ions exhibited a stronger promoting effect on aggregation via cation bridging than Na + ions. These findings reveal the synergistic regulatory effects of mineral type, protein coating, and environmental factors on microplastic-mineral heterogeneous aggregation, providing a theoretical foundation for predicting the transport and fate of microplastics in complex natural aquatic environments, as well as for developing biomolecule-based sustainable remediation strategies.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Xiaoxia Ye,Feiyang Wang,Juan Liu,Yifan Liu,Yuancai Lv,Chunxiang Lin,Liang Song,Minghua Liu,Ying Zhang,Jie Chen
Radioactive 137 Cs poses a severe threat in nuclear wastewater. Conventional powdered adsorbents suffer from poor recoverability and are ill-suited for large-scale continuous-flow operations. To address these limitations, a novel three-dimensional bulk ammonium phosphomolybdate-gelatin composite adsorbent (AMP@GA) was fabricated. Through this strategy, highly selective AMP particles were uniformly immobilized within a porous (92%) gelatin network. Rapid adsorption kinetics (reaching equilibrium within 30 min), a Langmuir-fitted theoretical maximum Cs + adsorption capacity of 142.17 mg·g −1 at 45 °C, and acceptable chemical stability across a broad pH range (2.0-11.0) were exhibited by the resulting AMP@GA. Most significantly, the material demonstrated outstanding selectivity over competing ions ( K d = 7.48 × 10 4 mL·g −1 ). Its practical viability was confirmed by achieving over 88% removal efficiency in authentic seawater. Furthermore, in fixed-bed column tests, the material sustained continuous operation for 163.5 h. The mechanism is dominated by NH 4 + -Cs + ion exchange, assisted by electrostatic interactions. This work presents a scalable, easily recoverable bulk adsorbent that effectively helps address the engineering bottlenecks of traditional powdered materials.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2026
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IF 7.9
Kunlin Chen,Lin Zhou,Jingyi Gu,Xiaolin Huang,Yaqi Zeng,Qingqi Wen,Jiale Yue,Chengshuai Liu,Weilin Huang,Qiaoyun Zeng,Chengyu Chen
Nanosized activated carbons (NACs) have emerged as promising adsorbents for antibiotic removal due to their excellent colloidal stability and low ecotoxicity. This study investigated four biomass-derived NACs for adsorption of oxytetracycline (OTC) and sulfamethoxazole (SMX). Both kinetic and isotherm analysis revealed higher affinity for OTC ( q max = 113.10–196.00 mg/g) than SMX ( q max = 60.66–124.90 mg/g), with adsorption capacity ranking NAC2 > NAC1 > NAC3 > NAC4. Adsorption was favored under mildly acidic conditions (pH 3–4) and at lower temperatures (20 ℃). Increased concentrations of NaCl and CaCl 2 enhanced antibiotic uptake through salting-out and complexation effects, respectively. Humic and fulvic acids significantly inhibited OTC adsorption due to steric hindrance but had minimal impact on SMX. Pore filling, hydrogen bonding, and π–π electron donor-acceptor interactions all contributed to adsorption. Density functional theory (DFT) calculations revealed that OTC had a lower HOMO-LUMO (highest occupied and lowest unoccupied molecular orbitals) energy gap (1.273 eV) and more negative binding energies (-63.5 to −182.2 kJ/mol) than SMX (2.013 eV; −47.1 to −158.2 kJ/mol), confirming its stronger chemical reactivity and affinity for NAC surfaces. The findings provide a comprehensive understanding of NAC-antibiotic interactions and demonstrate the potential of NACs for effective antibiotic remediation in aquatic environments.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
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IF 11.4
Rui Ding,Zhuozhi Ouyang,Xue Zhang,Yankai Dong,Xuetao Guo,Lingyan Zhu
Tire wear particles (TWPs) exposed to the aquatic environment are rapidly colonized by microorganisms and provide unique substrates for biofilm formation, which potentially serve as vectors for tetracycline (TC) to influence their behaviors and potential risks. To date, the photodegradation capacity of TWPs on contaminants due to biofilm formation has not been quantified. To accomplish this, we examined the ability of virgin TWPs (V-TWPs) and biofilm-developed TWPs (Bio-TWPs) to photodegrade TC when exposed to simulated sunlight irradiation. V-TWPs and Bio-TWPs accelerated the photodegradation of TC, with rates (kobs) of 0.0232 ± 0.0014 and 0.0152 ± 0.0010 h–1, respectively (kobs increased by 2.5–3.7 times compared to that for only TC solution). An important factor of increased TC photodegradation behavior was identified and linked to the changed reactive oxygen species (ROS) of different TWPs. The V-TWPs were exposed to light for 48 h, resulting in more ROS for attacking TC, with hydroxyl radicals (•OH) and superoxide anions (O2•–) playing a dominant role in TC photodegradation measured using scavenger/probe chemicals. This was primarily due to the greater photosensitization effects and higher electron-transfer capacity of V-TWPs in comparison to Bio-TWPs. In addition, this study first sheds light on the unique effect and intrinsic mechanism of the crucial role of Bio-TWPs in TC photodegradation, enhancing our holistic understanding of the environmental behavior of TWPs and the associated contaminants.
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JOURNAL OF HAZARDOUS MATERIALS
·
2026
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IF 10.6
Liang Zeng,Runji Ma,Xiaosong Gu,Jie Ou,Run Zhou,Junjian Wang
Pyrogenic carbon (PyC) is a ubiquitous redox-active material in natural and engineered environments, yet its environmental reactivity is commonly evaluated by measuring static electron-accepting and electron-donating capacities, without explicit consideration of electron transfer kinetics. Here, we developed a mediated electrochemistry–kinetic modeling framework that enabled simultaneous quantification of both equilibrium electron transfer capacities and intrinsic electron transfer rate constants for PyC in the aqueous phase, including both electron-accepting ( k A ) and electron-donating ( k D ) processes. Application of this approach to PyC produced at different pyrolysis temperatures revealed a tradeoff between capacity and kinetics, with high-temperature PyC exhibiting substantially faster electron transfer despite lower redox capacity. Reanalysis of more than 110 mediated electrochemical datasets from the literature demonstrated a general and robust trend of k A > k D across diverse PyC types. Structure–performance relationships integrating spectroscopic analyses and quantum chemical calculations identified carbon defects as the dominant drivers of electron transfer kinetics. Using p -nitrophenol as a model pollutant under anaerobic conditions, we showed that faster electron transfer kinetics enhanced degradation rates and favored oxidative transformation pathways. This study shifts the prevailing capacity-centric view of PyC redox reactivity toward a kinetics-driven framework and provides a mechanistic basis for predicting the role of PyC in aquatic environmental redox processes.
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高影响因子
Chemosensors
·
2023
·Vol. 11
·期 10
·531
·
IF 4.2
Mingzhu Wu,Jianhang Lin,Da Zheng,Yirui Yang,Zhihao Li,Zhengdong Zhu,Yonghui Shen,Gang Ni,Maofeng Zhang
Micro/nanoplastics are widespread in the environment and may cause severe damage to creatures and human beings. Micro/nanoplastic pollution has become a global focus issue; hence, the rapid and accurate detection of micro/nanoplastics is an essential step to ensure health. Herein, we report a surface-enhanced Raman scattering (SERS) technique to sensitively and quantitatively identify micro/nanoplastics in environmental water samples. A three-dimensional hierarchical Au@Ag nanostar (NSs) was synthesized and employed as an efficient SERS substrate. The “lightning rod effect” generated by tip branches of the nanostars and the coupling effect of the neighboring branches of the nanostar array enabled the ultra-trace detection of crystal violet (CV) down to 10−9M, even with a portable Raman device. Moreover, the hydrophobic property of the SERS substrate endowed it with a desirable enrichment effect, which meant an increase in the concentration or quantity of the micro/nanoplastic particles. And thereafter, the SERS sensor achieved a highly sensitive detection of polystyrene (PS) particle standard solution at a low concentration of 25 μg/mL or 2.5 μg/mL. Importantly, the detected concentration and the SERS intensity followed a nearly linear relationship, indicating the capability of quantitative analysis of micro/nanoplastics. In addition, the SERS sensor was successfully extended to detect PS particles in environmental water samples, including tap water, sea water, and soil water, and the detection concentration was determined to be 25 μg/mL, 2.5 μg/mL, and 25 μg/mL, respectively. The present Au@AgNSs array substrate with a two-order magnitude signal amplification further exhibited significant advantages in the label-free analysis of micro/nanoplastics in real water samples.Keywords:surface-enhanced Raman spectroscopy (SERS);Au@Ag nanostar;lightning rod effect;micro/nanoplastics;quantitative detection
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Surfaces and Interfaces
·
2025
·
IF 6.3
Hui Wang,Xuefei Wang,Ju Liu,Junru Li,Hongle An,Xiaodong Wang,Bingchun Xue
In this study, two Cu-doped covalent organic frameworks (Cu@COFs, namely Cu@TpBD and Cu@TpMDA) were successfully synthesized via the solvothermal method to address the challenge of bisphenol A (BPA) removal in aqueous systems. The adsorption behaviors of both Cu@COFs conformed to the pseudo-second-order kinetic model and the Langmuir isotherm model, indicating the monolayer chemisorption as the dominant mechanism. Notably, Cu@TpMDA exhibited a higher adsorption rate and a larger adsorption capacity for BPA compared to Cu@TpBD. This superior performance could be ascribed to the formation of Cu-O coordination bonds, which optimized the pore structure and enhanced the flexible features of Cu@TpMDA. The combination of characterization analyses, adsorption experiments, and density functional theory calculations revealed that the adsorption process was governed by a multi-synergistic adsorption mechanism, involving pore filling, hydrogen bond, π-π stacking, and metal coordination interaction. Remarkably, after five consecutive adsorption-desorption cycles, the BPA removal efficiencies remained over 97 % for Cu@TpMDA and 92 % for Cu@TpBD, confirming their excellent stability and reusability. The constructed coordination-driven flexible Cu@COFs system not only elucidates the structure-property-mechanism relationship, but also provides a theoretical framework for the targeted treatment of organic pollutants in complex aquatic environments.
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WATER RESEARCH
·
2024
·
IF 11.4
Yanlong Wang,Qinghui Zhao,Yuanfeng Guo,Shugang Hu,Guoqing Tian,Mengcheng Zhang,Xiaoqiang Cao,Huaqing Liu,Jian Zhang
The environmental transport and fate of nanoscale zero-valent iron particles (nZVI) in soil and groundwater can be altered by their hetero-aggregation with clay mineral particles (CMP). This study examines the interactions between bare or carboxymethyl cellulose (CMC)-coated nZVI with typical CMP, specifically kaolinite and montmorillonite. Methods include co-settling experiments, aggregation kinetic studies, electron microscopy, Derjaguin–Landau–Verwey–Overbeek (DLVO) and extended DLVO (EDLVO) energy analysis, and density functional theory calculations, focusing on the pH dependency of these interactions. The EDLVO theory effectively described the interactions between nZVI and CMP in aquatic environments. Under acidic conditions (pH 3.5), the interfacial interaction between bare nZVI and kaolinite is regulated by van der Waals forces, while complexation, van der Waals forces, and electrostatic attraction govern the interaction of bare nZVI with montmorillonite, primarily depositing on the Si O face. In contrast, the positively charged Al O face and edge of CMP are the main deposition sites for CMC-coated nZVI through hydrogen bonding, van der Waals forces, and electrostatic attraction. At neutral (pH 6.5) and alkaline (pH 9.5) conditions, both bare and CMC-coated nZVI predominantly attach to the Al O face and edge, facilitated by complexation or hydrogen bonding, alongside van der Waals forces. The attachment of CMC-coated nZVI to CMP surfaces shows reversible aggregation or deposition due to the steric repulsion from the CMC coating. These findings hold significant implications for the environmental applications and risk of nZVI.
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CHEMOSPHERE
·
2024
·
IF 8.1
Xinying Zhang,Yuling Zhang,Dong Li,Jili Wang,Yang Ding,Yiliang Wang,Liuyuan Feng,Yuliang Hu
In this study, we examined the aging characteristics of polyethylene (PE) and polylactic acid (PLA) microplastics (MPs), examining the adsorption behaviors and mechanisms concerning Cd(II) and Cr(VI) under both single and binary systems. The results revealed that aging treatment changed the physicochemical properties of MPs. The aging mechanisms of PLA and PE MPs were shown to be similar by the 2D-FTIR-COS study. These mechanisms involve the formation of oxygen-containing functional groups through the combination of carbon chain breakdown and oxygen. Aged MPs had a greater ability to adsorb metal ions than pristine MPs, with PLA MPs outperforming PE MPs. After 30 days of aging, Cd(II) adsorption increased by 40.61 % and 25.49 % for PE and PLA MPs, respectively, while Cr(VI) adsorption increased by 37.50 % and 69.29 %, respectively. The adsorption ability of PE and PLA MPs with Cd(II) or Cr(VI) under binary systems was less than that under single systems, with Cd(II) exhibiting more adsorption competitiveness than Cr(VI). Humic acid (HA), ionic species and strength , solution pH, and adsorption of Cd(II) and Cr(VI) were found to be significantly correlated. Further investigation into the adsorption mechanisms of Cd(II) and Cr(VI) on PE and PLA MPs revealed that pore-filling, electrostatic interactions , complexation, and hydrogen bonding play important roles in the adsorption process . The study's conclusions are crucial for assessing the risk associated with concurrent contamination by metal ions and microplastics.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Yongkai Lu,Tianxiang Ji,Wenjuan Xu,Dan Chen,Ping Gui,Feng Long
A definitive link between the micro- and nano-plastics (NPLs) and human health has been firmly established, emphasizing the higher risks posed by NPLs. The urgent need for a rapid, non-destructive, and reliable method to quantify NPLs remains unmet with current detection techniques. To address this gap, a novel laser-backscattered fiber-embedded optofluidic chip (LFOC) was constructed for the rapid, sensitive, and non-destructive on-site quantitation of NPLs based on 180º laser-backscattered mechanism. Our theoretical and experimental findings reveal that the 180º laser-backscattered intensities of NPLs were directly proportional to their mass and particle number concentration. Using the LFOC, we have successfully detected polystyrene (PS) NPLSs of varying sizes, with a minimum detection limit of 0.23 μg/mL (equivalent to 5.23 ×10 7 particles/mL). Moreover, PS NPLs of different sizes can be readily differentiated through a simple membrane-filtering method. The LFOC also demonstrates high sensitivity in detecting other NPLs, such as polyethylene, polyethylene terephthalate, polypropylene, and polymethylmethacrylate. To validate its practical application, the LFOC was used to detect PS NPLs in various aquatic environments, exhibiting excellent accuracy, reproducibility, and reliability. The LFOC provides a simple, versatile, and efficient tool for direct, on-site, quantitative detection of NPLs in aquatic environments.
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