JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jiaohui Xia,Yan Li,Xinbai Jiang,Dan Chen,Jinyou Shen
Electricity-stimulated anaerobic system (ESAS) has shown great potential for halogenated organic pollutants removal. Exogenous redox mediators can improve electron transfer efficiency to enhance pollutants removal in ESAS. In this study, humic acid (HA), a low-cost electron mediator, was added into ESAS to enhance the simultaneous reductive debromination and mineralization of 4-bromophenol (4-BP). Results showed that the highest 4-BP removal efficiency at 48 h was 95.43 % with HA dosage of 30 mg/L at − 700 mV, which was 34.67 % higher than that without HA. The addition of HA decreased the requirement for electron donors and enriched Petrimonas and Rhodococcus for humus respiratory. HA addition regulated microbial interactions, and enhanced species cooperation between Petrimonas and dehalogenation species ( Thauera and Desulfovibrio ), phenol degradation-related species ( Rhodococcus ) as well as fermentative species ( Desulfobulbus ). Functional genes related to 4-BP degradation ( dhaA/hemE/xylC/chnB/dmpN ) and electron transfer ( etfB/nuoA/qor/ccoN/coxA ) were increased in abundance by HA addition. The enhanced microbial functions, as well as species cooperation and facilitation, all contributed to the improved 4-BP biodegradation in HA-added ESAS. This study provided a deep insight into microbial mechanism driven by HA and offered a promising strategy for improving halogenated organic pollutants removal from wastewater.
研究领域:
环境工程
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微生物学
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生物修复
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Jiali Peng,Lun Li,Shihuai Deng,Hongyu Zhou,Yanjun Li,Chenye Fu,Long Lin,Yue Yuan,Wei Wei,Guochun Lv,Gang Yang,Xiaohui Lu,Bo Lai
Carbon nanotubes-driven persulfates oxidation processes (CNTs/PS) have been extensively studied for environmental remediation. Solution pH is one of the main factors affecting wastewater treatment, but it is often overlooked. Herein, we report the effect laws of pH on the mechanism of peroxymonosulfate (PMS) or peroxydisulfate (PDS) activation by CNTs. The oxidation of organics (e.g., phenol) in the CNTs/PDS system involves an electron transfer process mediated by metastable intermediates (CNTs−PDS*), whose potential is influenced by pH, reaching the highest oxidation potential under neutral condition. In the CNTs/PMS system, the active species (i.e., SO 4 •− , CNTs−PMS*) shifted with pH variations. In acidic environment, phenol oxidation is governed by CNTs−PMS* . As pH increases, PMS undergoes accelerated decomposition, generating SO 4 •− , which plays a crucial role in pollutant oxidation. Moreover, in the CNTs/PMS system, the oxidation products of phenol were not easily accumulated on CNT surfaces, contributing to a lower total organic carbon removal in solution. Additionally, the oxidation rates of phenolic compounds in the CNTs/PMS system, which involve more complex mechanisms, exhibited a weaker correlation with their descriptors (e.g., the octanol−water partition coefficient) compared to CNTs/PDS system. This comprehensive investigation deepens our understanding of CNTs/PS systems and provides guidance for selecting superior oxidants for wastewater treatment.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Huanji Song,Jiahao Sun,Lingshan Miao,Zhilong Lin,Shenghu Wang,Dongcheng Li,Weiyang Lv
Non-metallic catalysts have gained great attention in peroxymonosulfate based advanced oxidation processes (PMS-AOPs) for their enhanced safety and environmental compatibility. However, low catalytic efficiency, incomplete mineralization and harsh preparation methods still hinder their practical application. This work developed an innovative solvent-free ball milling-assisted pyrolysis strategy utilizing hexagonal boron nitride (h-BN) and multi-walled carbon nanotubes (MWCNTs) as synergistic precursors to construct the BN-CNT-700 composite. The mutually doped active sites were facilely formed through carbon/nitrogen hybridization , where electron-withdrawing C O groups dominated 1 O 2 generation while electron-donating C N sites primarily mediated SO 4 •− production. The radical and non-radical pathways worked in synergy to achieve complete removal of 20 mg·L −1 bisphenol A (BPA) coupled with an ultra-high mineralization efficiency of 88.6 %, surpassing most reported non-metallic counterparts and even outperforming various metal-based systems. Moreover, the BN-CNT-700/PMS system demonstrated exceptional environmental robustness, maintaining high BPA removal efficiency across broad pH ranges, various inorganic ions, and complex water matrices. This research offers the important implications for the rational design of non-metallic catalysts with tunable active sites for high-efficiency pollutant decontamination.
研究领域:
环境科学
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材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Zhaolei Zhang,Fengyan Fang,Pingping Zhang,Xiaokang Zhang,Hongchao Ma,Yanhui Wei
Efficient detection of 4- nitrophenol (4-NP) organic pollutant is always a very important issue due to the rapid development of chemical industry and the abuse of pesticides and so on. Here, we designed and synthesized a novel supramolecular fluorescent probe , 4-[4-(acetylamino)styryl]-1-cyclodextrin pyridinium p-toluenesulfonate (ASPT-β-CD), for the selective and sensitive detection of 4-NP. The introduction of β-CD not only improves the water solubility of probe and can also be used as a host to encapsulate 4-NP. In alkaline aqueous solution, the absorption spectrum of 4-NP overlaps the excitation spectrum of ASPT-β-CD and suggests that an internal filtration effect occurs between them. We explored the possible response mechanism and speculated that the high selectivity and high sensitivity were derived from the synergistic effect of inner filtering effect and host-guest interaction. Benefiting from the synergistic effect, the proposed sensor ASPT-β-CD displayed significant "turn-off" after adding 4-NP, while showing a fast response to 4-NP within 2 min and low LOD about 0.01 μM. In addition, this method has been successfully applied to the determination of 4-NP in lake water samples, indicating that the obtained ASPT-β-CD has great practical application potential in the environmental field.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Peng-Xu Yang,Jing Wang,Hui-Li Liu,Zhi-Yuan Guo,Zhi-Hui Huang,Pan-Pan Zhang,Zhi-Yong Ji
Inspired by the charge-governed protein channels located in the cell membrane, a series of polyether ether ketone-based polymers with side chains containing ionically cross-linkable quaternary ammonium groups and acidic groups have been designed and synthesized to prepare monovalent cation-selective membranes (MCEMs). Three acidic groups (sulfonic acid, carboxylic acid, and phenolic hydroxyl) with different acid dissociation constant (pKa) were selected to form the ionic cross-linking structure with quaternary ammonium groups in the membranes. The ionic cross-linking induced the nanophase separation and constructed ionic channels, which resulted in excellent mechanical performance and high cation fluxes. Interesting, the cation flux of membranes increased as the ionization of acidic groups increase, but the selectivity of MCEMs did not follow the same trend, which was mainly dependent on the affinity between the functional groups and the cations. Carboxyl group-containing MCEMs exhibited the best selectivity (9.01 for Li+/Mg2+), which was higher than that of the commercial monovalent cation-selective CIMS membrane. Therefore, it is possible to prepare stable MCEMs through a simple process using ionically cross-linkable polymers, and tuning acidic groups in the membranes provided an attractive approach to improving the cation flux and selectivity of MCEMs.
研究领域:
材料科学
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生物仿生学
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ANALYTICA CHIMICA ACTA
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2024
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IF 5.7
Yu Wang,Lingqi Shen,Yuan Yan,Bincheng Gong,Kexian Chen,Guohua Zhu,Zuguang Li
Background The use of pesticides to protect crops has long been an important measure to provide healthy and safe agricultural products, but excess pesticides flow into fields and rivers, causing environmental pollution. Earlier methods utilizing organic solvent liquid-liquid microextraction for pesticide residue detection were not environmentally friendly. Therefore, it is significant to find a greener and more convenient detection method to determine pesticide residues. Results A new method was established to detect three triazole fungicides (TFs), including myclobutanil, epoxiconazole and tebuconazole, in environmental water samples. And the determination was conducted using a high-performance liquid chromatography with the ultraviolet detector (HPLC-UV). The switchable deep eutectic solvent (SDES) can be reversibly switched between hydrophilic and hydrophobic states through temperature modulation. Additionally, the method exhibited excellent linearity for all target analytes within the concentration range of 10–2000 μg L −1 , with satisfactory R 2 values (≥0.9975). The limits of detection (LODs) ranged from 2.3 to 2.6 μg L −1 , and the limits of quantification (LOQs) ranged from 7.8 to 8.7 μg L −1 . The accuracy of the method was assessed through intra-day and inter-day precision tests, yielding relative standard deviations (RSDs) in the ranges of 2.8%–6.7% and 2.2%–7.5%, respectively. Density functional theory (DFT) results indicated that hydrogen bonding is a significant factor affecting the binding of DES with triazoles. Three different green assessment tools were used to prove that the SDES-HLLME method had good greenness and broad applicability. Significance This is a homogeneous liquid-liquid microextraction (HLLME) method based on the upper critical solution temperature (UCST) type switchable deep eutectic solvent program, which can complete the extraction within a few minutes without dispersant. In terms of pesticide detection, the analytical method is simple and more conducive to environmental protection.
研究领域:
环境科学
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分析化学
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PubMed
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2026
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IF 12.2
Yao Lu,Pin Wang,Hui-Xian Hu,Yu-En Guo,Shu-Xi Guo,Hua Li,Ye Du
The prechloramination followed by ozonation (NH2Cl–O3) process effectively mitigates bromate (BrO3–) formation in bromide-containing waters but inadvertently enhances the production of halogenated and nitrogenous disinfection byproducts (DBPs). Cytotoxicity assays revealed that the presence of precursors such as L-tyrosine (Tyr), L-tryptophan (Trp) and tannic acid during the NH2Cl–O3 process contributed to this increase in nitrogenous and halogenated DBPs and resulted in elevated overall toxicity. Nontargeted ultrahigh performance liquid chromatography-Orbitrap tandem mass spectrometry identified diverse halogenated DBPs, with NH2Cl–O3 yielding up to 5-fold more structures and higher abundances than NH2Cl or O3 alone. Taking Tyr as an example, proposed DBP (4-bromophenol, 4-hydroxyphenylacetamide, etc.) formation pathways, involving haloamine-mediated N-halogenation, O3-driven oxidation, decarboxylation, and deamination, were supported by density functional theory (DFT) calculations, confirming both thermodynamic and kinetic feasibility. Matrix-dependent quantitative validation in Suwannee River humic acid (SRHA) and wastewater effluents showed that concentrations of some identified DBPs reached tens of μg/L, dominated by aromatic halo-phenolics and brominated derivatives. In silico quantitative structure–activity relationship (QSAR) models and cytotoxicity assays indicated that these aromatic halo-DBPs exhibited comparable toxicities to conventional DBPs (e.g., dichloroacetonitrile, N-nitrosodimethylamine), but had a higher toxicity index than BrO3–. These findings highlight trade-offs in water disinfection, underscoring the need for optimized strategies to co-control BrO3– and toxic organic DBPs.
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高影响因子
Nature Communications
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2026
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IF 18.1
Wang Jiachen,Li Jinxin,Xie Mengjiao,Quan Xie,Liu Yanbiao
The electrocatalytic upcycling of halogenated pollutants into value-added chemicals presents a sustainable frontier, yet precise transformation pathways remain challenging. Here, we report a pulsed electrocatalytic strategy that exploits a temporal modulation to realize a dynamic coordination mechanism, enabling the sequential conversion of 4-chlorophenol (4-CP) to para -benzoquinone ( p -BQ) over an N, O-dual coordinated Fe single-atom catalyst (FeN 2 O 2 SAC). Diverging from conventional continuous electrolysis, pulsed catalysis spatiotemporally decouples cathodic dechlorination and anodic oxidation, exerting precise control over transient intermediate populations. In situ spectroscopy and density functional theory reveal that pulse polarization drives a dynamic chloride-coordination process at the Fe center. This transient ligand-field modulation optimizes the adsorption energetics and lowers the thermodynamic barrier. Consequently, the FeN 2 O 2 SAC achieves a 4-CP conversion of 94.8% and a p -BQ yield of 62.6%, outperforming the FeN 4 architecture. This system demonstrates long-term durability in flow electrolyzers alongside a reduced carbon footprint. By coupling pulsed electrocatalysis with dynamic coordination chemistry, this work establishes a paradigm for “pollutant-to-product” conversion, offering a scalable blueprint for circular chemical economies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Dazhen Xiong,Huihui Ma,Jiaming He,Yijie Han,Wenjie Ma,Cailing Wu,Yunlei Shi,Zhiyong Li,Huiyong Wang,Yang Zhao,Jianji Wang
High-performance soft materials with stimulus-responsive and self-healing properties have received a lot of attention in modern environmental and energy technologies. However, it was difficult to construct supramolecular hydrogels integrating different functionalities. In this work, we reported a novel class of supramolecular hydrogels made of ionic liquids (ILs) with CO 2 -responsive and self-healing properties. These ILs were found to form hydrogels with H 2 O. Upon bubbling with CO 2 , the transparent and stable IL-based hydrogels transformed into sols, which returned to their initial gel state after bubbling with N 2 at 65°C. The reversible gel-sol phase transformation behavior was demonstrated by rheological, polarizing, scanning and cryogenic transmission electron microscopy measurements. Spectroscopic studies indicated that the mechanism of gel-sol transition was attributed to reversible reaction between the anions of the ILs and CO 2 in the hydrogel, which destroyed the hydrogen bonding between the anions and water. Self-healing ability of the hydrogels was confirmed by rheological measurements. The self-healing mechanism was ascribed to the disruption and reconstruction of hydrogen bonds in IL-based hydrogels using temperature-dependent Fourier transform infrared spectroscopy. The CO 2 -responsive and self-healing ability make these novel hydrogels attractive in smart soft materials.
研究领域:
材料科学
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化学工程
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PubMed
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ACS Catalysis
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2024
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IF 11.3
Yunjia Wei,Dexiang Chen,Xingce Fan,Xiao Tang,Lei Yao,Xing Zhao,Qiang Li,Jiawei Wang,Teng Qiu,Qi Hao
The Suzuki–Miyaura coupling reaction is an efficient organic method for synthesizing biphenyl products. However, its conventional reliance on toxic soluble organometallic palladium catalysts or expensive palladium nanoparticles, along with the need for elevated temperatures and prolonged reaction times, presents a significant challenge. Herein, we demonstrate a palladium-free approach using plasmonic silver nanoparticles that enables the Suzuki–Miyaura coupling reaction to proceed at room temperature under visible light. Utilizing the surface-enhanced Raman scattering characteristics of silver, we conducted dynamic self-monitoring of the reaction. Our findings reveal that this plasmon-induced Suzuki–Miyaura coupling reaction fundamentally operates as a heterogeneous reaction involving coupling between radicals, distinct from conventional palladium-based reactions. Moreover, the cleavage of C–Cl and C–B bonds, fundamental prerequisite to the coupling, is driven by plasmonic hot electrons and plasmon-induced reactive oxygen species, respectively. These findings not only provide insights into the design and regulation of plasmonic catalysts but also enhance theoretical understanding of the Suzuki–Miyaura reaction in a broader context.
研究领域:
化学
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材料科学
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光催化
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DOI
高影响因子
Nature Water
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2025
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IF 24.1
Shi Lu-Jia,Huang Gui-Xiang,Wang Zhao-Hua,Duan Yanghua,Zhang Ying-Jie,Chen Jie-Jie,Li Wen-Wei,Yu Han-Qing,Elimelech Menachem
Non-radical oxidation of pollutants by direct electron transfer has gained heightened interest in water purification for its higher selectivity and efficiency and lower tendency for byproduct formation than traditional advanced oxidation processes. Engineering of catalysts for efficient activation of two substrates (that is, pollutant and oxidant) is essential to trigger the direct electron transfer reactions but is often hindered by the distinct properties of the co-present substrates. We investigated the individual interaction between the catalyst and each substrate and proposed a dual-substrate synergistic catalysis strategy to achieve separate optimization of each substrate activation process. Experimental and theoretical analyses reveal a strong synergistic effect between the two catalysts that preferentially activate the substrates and have smaller resistance for interfacial electron transfer, thus drastically improving the decontamination efficiency. The dual-substrate synergistic catalysis system offers a conceptual advancement in achieving green and efficient water purification by substrate-specific activation, facilitating flexible design and mechanistic exploration of complex heterogeneous catalytic processes.
研究领域:
环境科学
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催化化学
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水处理技术
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Baoquan Liu,Lianchong Shao,Jiayun Yu,Feipeng Huang,Chengpu Chu,Shaoping Tong,Laiquan Li,Huan Wu,Yinghua Xu,Bin Liu
Halogenated disinfection byproducts (DBPs) pose significant health risks owing to their widespread occurrence and high toxicity in drinking water. Traditional water treatment technologies often fail to remove these toxic compounds without generating secondary pollutants. Herein, we report a sustainable and highly efficient electrochemical hydrogenation (ECH) strategy using a delicately designed ruthenium nanoparticle-modified electrochemical‑hydrogen-membrane (Ru NPs-EHM) reactor, which enables the complete conversion of halogenated DBPs into non-toxic products without the need for supporting electrolyte. The reactor achieves >99.9% conversion of 12 representative halogenated DBPs, with minimal formation of hazardous intermediates. The exceptional catalytic performance is attributed to the strong adsorption capability of Ru nanoparticles and the unique EHM configuration, which enhances both ECH selectivity and efficiency. This work presents a breakthrough in water treatment technology, offering a cost-effective, environmentally friendly, and scalable solution for the safe purification of drinking water.
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