JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yibin Yang,Rui Chen,Zhiqiang Zhang,Yuke Qin,Attiqa Parveen,He Bai,Xiaoqiang Jia
Phenanthrene, a pervasive polycyclic aromatic hydrocarbon (PAH), poses significant environmental and health risks due to its persistence and bioaccumulation. This study presents the development of a synthetic bacterial consortium comprising three engineered Escherichia coli BL21(DE3) strains, each harboring distinct catabolic modules encoded by pET-28(a) plasmids for the complete mineralization of phenanthrene. The consortium was engineered by integrating 17 genes critical for phenanthrene degradation, organized into three distinct modules that harness the collective metabolic potential of separate strains to enhance the degradation process. Each module was tailored to a specific phase of phenanthrene catabolism, ensuring the coordinated and efficient breakdown of the pollutant. Following the identification of rate-limiting enzymes within the up- and downstream degradation modules, the eight corresponding genes were subjected to laboratory evolution using the SCRaMbLE method to bolster the degradation capabilities of the strains. The consortium was then tested in a minimal salt medium (MSM) containing 100 mg/L phenanthrene. Following their evolution, the two SCRaMbLE strains E. coli SCRPHE033 and E. coli SCRKA065 exhibited enhanced degradation rates of 11.5 and 25.18 % for their respective substrates. Finally, the comprehensive phenanthrene degradation system, which includes the two SCRaMbLE strains and E. coli CRSA, was subjected to comprehensive optimization, after which it achieved a significant degradation efficiency of 84.33 % for 100 mg/L phenanthrene within a 120-hour timeframe. This research demonstrates the potential of synthetic biology in constructing microbial consortia for environmental bioremediation based on the SCRaMbLE method, offering a promising strategy for mitigating PAH pollution.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Na Zhang,Lei-qiang Liu,Yao Zhang,Jun Shen,Yu-gao Wang,Gang Liu,Yan-xia Niu
Coal tar pitch (CTP) is a carbon material with abundant yield in China, but the toxic polycyclic aromatic hydrocarbons (PAHs) contained in it have restricted its broader applications. In order to reduce the PAHs content, an alkylation method was developed in this study to modify CTP (MCTP) by using 1-dodecene as the alkylating reagent, and the optimal reaction conditions (temperature 170 °C, time 4 h, solvent dosage 60 times that of CTP, and alkylating reagent dosage 4 times that of CTP) for synthesizing the MCTP were determined by alkylation modification with model compounds. Compared with CTP, the content of PAHs in MCTP was reduced by 97.35 %. The mechanism of the reaction was explained by analyzing the types of alkylation products and combining structural analyses of CTP and MCTP. PAHs emissions from fumes and the toxic equivalent quantity (TEQ) among different environmental standards were greatly reduced, while MCTP demonstrated low cytotoxicity and ecotoxicity. The method can also be applied to the toxicity assessment of road materials such as alkylation by-products.
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Asia-Pacific Journal of Chemical Engineering
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2025
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IF 1.6
Zhiwei Shi,Xinyu Jia,Hao Chen,Yagang Zhang,Xinfu He,Anning Zhou,Mingyi Wang
Aromatics and hydrogenated aromatics constitute the primary constituents of the recycled solvent utilized in coal liquefaction. However, the presence of hydrogenated aromatics complicates the assessment of the effects of aromatic compounds during the coal liquefaction process. To eliminate the effect of hydrogenated aromatics, solvent-free experiments and experiments with specific polycyclic aromatic compounds (pyrene, fluoranthene, phenanthrene, and naphthalene) were conducted, along with utilizing density functional theory calculations. Results show that the shuttle role of naphthalene is influenced by catalyst activity. In the presence of a low-active catalyst, naphthalene acts as a shuttle agent facilitating indirect hydrogen transfer. However, with a high-active catalyst, direct transfer of hydrogen from H 2 to pyrolysis radicals occurs without involving naphthalene as an intermediary. Polycyclic aromatic compounds exhibit higher hydrogen shuttle ability (pyrene > fluoranthene > phenanthrene > naphthalene). The high hydrogen shuttle ability can be attributed to the higher reactivity in hydrogenation and lower energy barriers for hydrogen transfer. A nonradical hydrogen transfer pathway has been proposed, promoting cleavage of strong covalent bonds and enhancing the yield of asphaltene and preasphaltene. Additionally, π–π inter actions between polycyclic aromatic compounds and pyrolysis radicals have been evaluated. The interactions contribute positively to radical stability. Substances characterized by a greater number of aromatic rings display a more pronounced stabilizing effect on free radicals.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yarui Zhou,Xin Xiao,Zilong Li,Bei Zhang,Baoliang Chen
Nano zero-valent nickel nanoparticles (Ni 0 NPs) were successfully immobilized onto Enteromorpha -derived biochar to enhance the removal of polycyclic aromatic hydrocarbons (PAHs) from aqueous solutions through an integrated adsorption-magnetic recovery process. Comprehensive characterization techniques revealed the uniform dispersion of Ni 0 NPs on the biochar surface, with particle sizes predominantly ranging from 60 to 100 nm. The synthesized composites (HTNF@Ni 0 ) exhibited an exceptional specific surface area of 1388 m 2 /g, which contributed to its outstanding phenanthrene removal performance, achieving a maximum adsorption capacity of 248.54 mg/g. The experimental data were well-fitted by pseudo-second-order kinetics and Langmuir isotherm adsorption model. Moreover, the magnetic composite demonstrated excellent regeneration properties and stability in phenanthrene removal after four consecutive cycles. Additionally, the optimized structure, charge distribution, LUMO-HOMO energy gap (E GAP ), and adsorption energy of the composite indicated strong π-π interactions and charge transfer between active functional groups (e.g., –OH, −NHR, –COOH, −C–OH), particularly the electron donor–acceptor interaction between metallic Ni 0 nanoparticles and target contaminants. The interaction was confirmed as an exothermic process, predominantly governed by chemical adsorption mechanisms. This study provides novel insights into the development of innovative magnetic composites and their potential for practical applications in wastewater treatment.
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Journal of Water Process Engineering
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2025
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IF 6.7
Xianxian Sheng,Meesam Ali,Ruoxuan Xu,Mudassir Habib,Xiang Zhang,Qian Sui,Rongbing Fu,Shuguang Lyu
Mackinawite (FeS) is a promising catalyst for advanced oxidation processes (AOPs), but its role in activating sodium percarbonate (SPC)-dominated oxidation remains unclear. Herein, citric acid (CA) was introduced as a synergistic agent to enhance FeS activation of SPC, demonstrating that SPC/FeS and SPC/CA systems hardly removed 6.8 % and 7.6 % of fluoranthene (FLT), respectively, while SPC/FeS/CA process achieved a significant 96.2 % FLT degradation. Reactive oxygen species (ROS) analysis identified HO and O 2 − as the dominant contributors to FLT degradation. X-ray photoelectron spectroscopy (XPS) confirmed that S(-II) facilitated the Fe(III)/Fe(II) redox cycle, ensuring prolonged FLT degradation, which was further confirmed through Na 2 S experiments. GC–MS identified benzoic acid (BA) and phthalic acid (PA) as degradation intermediates with reduced toxicity than FLT, highlighting the environmental safety of the proposed technique. SPC/FeS/CA system effectively mitigated the inhibitory effects of neutral to weakly alkaline pH conditions (8.0–10.0) and achieved significant FLT degradation (60.7 %) even at pH 11.0. In soil slurry experiments, the process removed 80 % of FLT within 12 h. The system effectively degraded other polycyclic aromatic hydrocarbons (PAHs), including naphthalene and phenanthrene, demonstrating its broad applicability for remediating PAHs-contaminated environments. This study introduces a novel SPC-dominated AOP strategy, leveraging FeS as a robust catalyst, and offers valuable insights for advancing efficient PAHs remediation technologies.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Xue Ma,Mengmeng Fu,Kai Hu,Li Gao,Chenchen Song,Shusheng Zhang,Renyong Zhao,Wenjie Zhao
Developing efficient and reliable adsorbents with simplified synthesis and mixed-mode performance is crucial for the accurate quantitative analysis of diverse coexisting environmental pollutants. A magnetic carboxylated hypercrosslinked organic polymer (Fe 3 O 4 /HCP-COOH) with reverse phase/cation exchange mixed-mode performance was synthesized through a two-stage process: (1) Fabrication of HCP-COOH via FeCl 3 -catalyzed Friedel-Crafts alkylation using 1,4-phenylenediacetic acid and 1,4-bis(chloromethyl)benzene; (2) In situ growth of Fe 3 O 4 nanoparticles on HCP-COOH through coprecipitation, utilizing FeCl₃ dually as polymerization catalyst and iron precursor to enhance process efficiency and waste minimization. The nanocomposite functioned as a mixed-mode sorbent for magnetic solid-phase extraction (MSPE), integrating dual retention mechanisms to selectively extract hydrophobic polycyclic aromatic hydrocarbons (PAHs) and cationic quaternary ammonium pesticides (QUATs), with subsequent analysis by GC-MS for PAHs and HPLC-MS/MS for QUATs respectively. Following optimization of adsorption pH, eluent composition, and contact time, the method exhibited high sensitivity with limits of detection (LODs) of 0.80-7.93 ng L⁻¹ for 15 PAHs and 0.02-16.31 ng L⁻¹ for 4 QUATs. Validation showed satisfactory recoveries of 89.5-98.3% (RSDs ≤11.2%) in snowmelt and 90.4-101.8% (RSDs ≤11.6%) in lake water (n=3), confirming practicality for simultaneous monitoring of hydrophobic and cationic contaminants in complex environmental water, offering significant advantages in multi-residue analysis for environmental monitoring applications.
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ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Runnan Zhang,Yanyan Liu,Wanqi Ou,Yuying Ye,Kai Xu
Polycyclic Aromatic Hydrocarbons (PAHs) are persistent organic pollutants that are widely present in aquatic environments and pose a significant threat to the ecological environment and human health. This study introduces a novel magnetic biochar-supported metal oxide catalyst (CeO 2 /BC@Fe 3 O 4 , CBF) as a peroxymonosulfate (PMS) activator in phenanthrene (PHE) degradation in aqueous environments. The degradation performance of the CeO 2 /BC@Fe 3 O 4 composite material was investigated through degradation experiments. The results showed that under the optimal reaction conditions, the degradation efficiency of 20 mg/L PHE solution within 60 minutes could reach 99.55% and maintained stability within a wide range of pH values. Radical quenching and EPR studies confirmed the involvement of SO 4 ·- , ·OH and 1 O 2 in the removal of PHE during the degradation process. The possible degradation pathways were proposed based on the identification of intermediates. The catalyst demonstrated excellent reusability and was effective in real water samples and for other organic pollutants, highlighting its potential for practical environmental applications.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Han Gao,Shang Gao,Lei Wang,Zhen Song,Xiaolei Qu,Minli Wang,Tao Long,Jinzhong Wan
Thermal treatment is a commonly applied soil remediation technique that can also change the properties of soil. However, few studies looked into the transformation and mechanism of soil organic matter (SOM) at the molecular level when contaminated soil undergoes thermal remediation. Herein, FT-ICR MS, pyrolysis gas chromatography mass spectrometry (Py-GC–MS), and size exclusion chromatography-diode array detector-fluorescence detector-organic carbon detector (SEC-DAD-FLD-OCD) were used to unveil the molecular transformation mechanism of SOM under 100 °C and 400 °C treatments. The macromolecules transformed to humic and fulvic components after 400 °C treatment, while few transformations occurred after 100 °C treatment. The molecules decreased with the increase in temperature. After 400 °C treatment, over 99 % of the molecules were newly produced, which were mainly aromatic (66 %) and lignin-like (19 %) components. After 100 °C treatment, most of the molecules (73.6 %) were reserved. The unsaturation and aromatic structures of SOM increased significantly after the 400 °C treatment, while the changes were relatively minor after the 100 °C treatment. The fracture of the carbon skeleton, cyclization, and H abstraction reactions were the main mechanisms for the molecular transformation of SOM during 400 °C treatment, while volatilization was the main transformation scheme during 100 °C. Statistical results of pyrolysates show the increase of aromatic components, and the molecular markers reflected the increase of condensed organic carbon and the decrease of phenols, alkene components during 400 °C treatment. The sorption of PAHs for soil decreased after treatment, owing to the loss and transformation of SOM. This study advances the mechanistic understanding of transformation in SOM molecular signatures during thermal treatment.
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Environmental Science-Nano
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2025
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IF 5.1
Menghan Cui,Jin Zhang,Chenghao Huang,Shuangyuan Xu,Bożena Czech,Jianggang Han,Yu Shen,Xinhua Zhan
Polycyclic aromatic hydrocarbons (PAHs) are persistent organic pollutants that pose significant risks to the environment and human health. Phenanthrene (PHE), a model PAH, has been shown to cause toxic effects on plants, particularly on their photosynthetic performance. This study investigated the potential of nano-biochar (nBC) derived from rice straw to alleviate the phytotoxicity of PHE in wheat seedlings. We hypothesized that the high adsorption capacity and unique properties of nBC, such as its high surface area, porous structure, and abundant functional groups, could reduce the bioavailability and toxicity of PHE, thereby mitigating its adverse effects on wheat growth and photosynthesis. Wheat seedlings were exposed to different treatments, control, 1.0 mg L−1 nBC, 1.0 mg L−1 PHE, 1.0 mg L−1 PHE + 0.5 mg L−1 nBC, and 1.0 mg L−1 PHE + 1.0 mg L−1 nBC. The results showed that nBC alleviated PHE-induced chlorosis and improved plant growth. Compared to the PHE-single treatment, the application of 1.0 mg L−1 nBC increased chlorophyll content by 14.54% and enhanced photosynthetic efficiency, as evidenced by increases in Fv/Fm (2.48%), qP (9.06%), and ΦPSII (3.81%). Furthermore, nBC reduced the accumulation of PHE in wheat tissues, with the PHE concentration in the PHE-single treatment being 1.77 and 1.61 times higher than that in the 1.0 mg L−1 nBC treatment for shoots and roots, respectively. The non-photochemical quenching (NPQ) values decreased by 13.64% in the presence of 1.0 mg L−1 nBC, indicating reduced heat dissipation and improved photosynthetic performance. The alleviation of PHE toxicity by nBC can be attributed to its high adsorption capacity, which limits the uptake of PHE by plants. Additionally, the photoelectric effect of nBC may directly promote photosynthesis by enhancing electron transport and providing reducing power for ATP and NADPH synthesis. The use of nBC for the remediation of PAH-contaminated soils offers several advantages, including sustainability, eco-friendliness, and additional benefits such as carbon sequestration and soil quality improvement. These findings highlight the potential of nBC as an effective amendment for the remediation of PAH-contaminated soils and the protection of crops under PAH stress.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xudong Zhang,Yang Deng,Yanhua Liu,Fan Yang,Yugao Wang,Jun Shen
Carbazole is a highly value-added compound derived from crude anthracene. Deep eutectic solvents (DESs) have been extensively used as promising green solvents for the separation of target compounds from mixture. In this work, 135 acidic DESs, formed by combining 9 quaternary ammonium salts with 15 common acids, were screened based on the conductor-like screening model for real solvents (COSMO-RS) model. The four top-ranked DESs, including tetraethylammonium chloride (TEAC)/2 acetic acid (AA), TEAC/2 propionic acid (PA), tetrapropylammonium chloride (TPAC)/2AA, and TPAC/2PA were identified as suitable extractants for carbazole separation based on their performance index (PI). Among them, TEAC/2AA had the best separation performance for carbazole due to its highest PI value (1448.19). Liquid–liquid extraction experiments were performed, and the results were in good accordance with those predicted by COSMO-RS calculations. Therefore, TEAC/2AA was determined as the most promising DES for the carbazole separation. The extraction conditions of TEAC/2AA were optimized. The extraction efficiency (EE) and selectivity (SE) of carbazole were 97.67 % and 66.64 %, respectively, under the optimal extraction conditions (25 ℃, 5 min of extraction time, DES-oil mass ratio of 1:5, initial carbazole concentration of 5000 ppm). Additionally, the deionized water was employed to regenerate the DES and recovery of carbazole. The recycling performance of promising DES was also investigated. Finally, quantum chemical calculations and Fourier Transform Infrared spectroscopy (FT-IR) analysis were conducted to explore the separation mechanism. The results indicated that the separation of carbazole by DESs were predominantly dominated by hydrogen bonds and van der Waals interaction. This work provided a valuable reference for the selection and design of DES extractants to separate other high value-added components from mixture.
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INTERNATIONAL MICROBIOLOGY
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2024
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IF 2.3
Zhang Mingle,He Zhimin,Xu Xiaoyi,Ji Fan,Wang Bin
This study investigates the advantages of combined microbial degradation of polycyclic aromatic hydrocarbons (PAHs) in reducing the inhibitory effects of high-concentration eluents commonly used in soil washing. A microbial synergistic strategy was proposed using Arthrobacter sp. SZ-3 and Pseudomonas putida B6-2 as the key bacteria in the presence of Tween 80. The results show that in systems with Tween 80, the SZ-3 strain exhibits a strong capacity to degrade three types of PAH compounds, while the B6-2 strain follows multiple degradation pathways. Mixed bacteria achieved degradation rates 60.70% higher than single bacteria at varying concentrations of Tween 80. Additionally, the average growth rates of mixed bacteria increased by 1.17–1.37 times, aligning with the changes in the functional group. Protein activity detection within each degradation system corresponded with growth quantity and the cyclic variation characteristics of ETS enzyme activity. Notably, the ETS activity of mixed bacteria was 150% higher than that of single bacteria. At a Tween 80 concentration of 500 mg/L, the degradation rates of PAHs (Phe, Flu, Pyr) by mixed bacteria were significantly higher than those by single bacteria. The catechol 1,2-dioxygenase activity of mixed bacteria was 2.30 times higher than that of single bacteria. While Tween 80 did not alter the PAH degradation pathways, it significantly influenced the accumulation amount and duration of the characteristic intermediate product. This provides a reference for the remediation of recalcitrant pollutants under conditions involving high-concentration surfactants.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Chunyan Liu,Yanjuan Liu,Yuefei Zhang,Wei Chen,Sheng Tang
In this work, zeolitic imidazolate framework-67 (ZIF-67) with excellent stability synthesized at room temperature was used together with amphiphilic polymer hydrogel to synthesize a captivating mixed-mode silica stationary phase for the first time. The amphiphilic polymer hydrogel prepared by weakly basic cationic and acidic anionic monomers that was modified on the surface of ZIF-67@SiO 2 by a simple physical coating method not only improved the separation performance, but also enhanced the applicability of ZIF-67@SiO 2 in chromatographic analysis. Meanwhile, the porous ZIF-67 effectively alleviated the problem that polymer hydrogel was easy to swell. To sum up, the amphiphilic polymer hydrogel and ZIF-67 showed excellent synergistic effect in improving the separation ability and the applicability of stationary phase. The experimental results demonstrated that the ZIF-67/hydrogel@SiO 2 stationary phase could be applied in various chromatographic separation modes, demonstrating superior resolution and separation selectivity for polycyclic aromatic hydrocarbons, steroid hormones, nucleosides, B-vitamins, sulfonamides, benzoic acids and dinitrobenzene isomers. In this study, the synergistic expression of ZIF-67 and polymer hydrogel provided a new idea for the development of silica stationary phase co-modified by metal-organic framework and hydrogel material. Concurrently, the successful preparation of ZIF-67/hydrogel@SiO 2 composite revealed a new possibility for utilizing ZIF-67 as the functional material of stationary phase, expanding the application potential of ZIF-67 in the field of chromatography.
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