JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Suhang Wang,Jiaqing Liang,Yongkai Liao,Haixuan Zhou,Brian J. Reid,Chao Cai
The biodegradation of polycyclic aromatic hydrocarbons (PAHs) involves complex metabolic interactions among multiple degradation pathways. However, how interactions among different pathways influence the overall degradation efficiency remains poorly understood. In this study, Pseudoxanthomonas sp. G3, an efficient degrader of phenanthrene (PHE) and pyrene (PYR), was used to investigate pathway interactions under mixed-PAH conditions. Genomic and metabolomic analyses revealed that strain G3 degrades PHE and PYR through three pathways: the phthalate pathway (with phthalic acid as the dead-end product), a shared catechol degradation pathway, and the benzoate degradation pathway. Notably, PYR induced the benzoate degradation pathway, representing a previously unreported metabolism of PYR by bacteria. Integrated analyses revealed that PHE inhibits PYR degradation via dual mechanisms. Specifically, PHE preferentially utilizes the PYR-induced benzoate degradation pathway, thereby diverting metabolic flux and impeding PYR degradation. Moreover, the benzoate degradation pathway further inhibits the catechol degradation pathway, intensifying suppression of PYR degradation. These findings elucidate mechanistic insights into the interactions among the biodegradation pathways under mixed-PAH stress and provide a theoretical basis for targeted improvement of the efficiency and predictability of mixed-PAH degradation.
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY
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2026
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IF 4.2
Pengrui Zhang,Haiyang Zhang,Xinyu Yang,Yuanli Wu,Shanshan Dai,Yanqin Ding,Shanshan Sun
Bacteria play an important role in the biodegradation of polycyclic aromatic hydrocarbons (PAHs), especially the more recalcitrant high-molecular-weight compounds like pyrene. In this study, we isolated and characterized a novel pyrene-degrading bacterium, Glutamicibacter soli ENR6, from petroleum-contaminated soil. Strain ENR6 was able to utilize various PAHs as sole carbon sources and degrade 88.8% of 50 mg L−1 pyrene and 76.8% of 100 mg L−1 pyrene within 15 days. During pyrene degradation, eight metabolites were detected, with 2,2′-diphenic acid emerging as the predominant intermediate. By day 7, 40.6% of the degraded pyrene had accumulated in the form of 2,2′-diphenic acid, which was subsequently metabolized via the phthalate pathway. To our knowledge, this is the first report identifying 2,2′-diphenic acid as an intermediate in pyrene degradation. Integrated genomic and transcriptomic analyses revealed four gene clusters (clusters I–IV) involved in pyrene degradation in strain ENR6. Reverse transcription-quantitative PCR (RT-qPCR) analysis demonstrated that these clusters were specifically induced by pyrene and its intermediates, with genes chr_3400-chr_3404 in cluster I strongly associated with 2,2′-diphenic acid degradation. Based on these findings, we propose a distinct 2,2′-diphenic acid-centered pathway for pyrene degradation in strain ENR6. This study not only broadens the bacterial repertoire available for PAH bioremediation but also provides new insights into the metabolic diversity of PAH-degrading microorganisms.
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Ruomu Chen,Yumeng Niu,Nan Li,Jingrui Peng,Ziqian Xia,Chenyang Wang,Jiandong Jiang,Kai Chen
Nitro-polycyclic aromatic hydrocarbons (nitro-PAHs) are toxic and persistent environmental contaminants of increasing concern because of their widespread occurrence and ecological risks. Nitronaphthalene, a representative nitro-PAH, occurs as positional isomers, yet microbial degradation studies have mainly focused on 1-nitronaphthalene (1-NN), leaving the basis for biodegradation of 2-nitronaphthalene (2-NN) largely unresolved. In this study, Burkholderia pseudomultivorans M3 was isolated from river sediment in Anhui Province, China, and was found to efficiently degrade both 1-NN and 2-NN, indicating an expanded degradation range for nitronaphthalene isomers. Genome analysis identified a novel nitronaphthalene degradation gene cluster ( nnd ) that is phylogenetically related to reported nin - and nag -type gene clusters but differs functionally from both. Gene knockout and complementation experiments demonstrated that nndAc , encoding the catalytic α-subunit of a Rieske-type dioxygenase, is essential for degradation of both isomers. Heterologous expression and metabolite identification further showed that the NndAB system transforms 1-NN and 2-NN into 1,2-dihydroxynaphthalene via the corresponding nitro-dihydrodiol intermediates, with concomitant nitrite release. Site-directed mutagenesis revealed that the ability of NndAc depends on the coordinated effects of multiple active-site residues, with F200 being particularly important for 2-NN transformation. Moreover, strain M3 maintained substantial removal efficiency in synthetic wastewater containing mixed nitro-, carboxyl-, and hydroxyl-substituted naphthalene compounds, supporting its applicability in complex contaminated matrices. These findings reveal the molecular basis underlying the broadened substrate range of nitronaphthalene degradation and highlight the potential of strain M3 for remediation of wastewater containing mixed substituted naphthalene pollutants.
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ACS Synthetic Biology
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2021
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IF 5.11
Guangbao Zhang,Xiaohui Yang,Zhenhua Zhao,Tao Xu,Xiaoqiang Jia
Polycyclic aromatic hydrocarbons (PAHs) are highly toxic and persistent organic pollutions that can accumulate in the environment. In this study, an aromatic ring cleavage module, a salicylic acid synthesis module, and a catechol metabolism module were respectively constructed in three Escherichia coli BL21 strains. Subsequently, the engineered strains were cocultured as an artificial consortium for the biodegradation of phenanthrene, a typical PHA. Single factor experiments and response surface methodology were used to identify the optimal degradation conditions, including an inoculation interval of 6 h, inoculation ratio of 1:1:1, and IPTG concentration of 2 mM. Under these conditions, the 7-day degradation ratio of 100 mg/L phenanthrene reached 72.67%. Moreover, the engineered Escherichia coli BL21 strains showed good phenanthrene degradation ability at substrate concentrations 10 mg/L up to 500 mg/L. Enzyme activity assays combined with gas chromatography–mass spectrometry measurements confirmed that the three engineered strains behaved as a synergistic consortium in the phenanthrene degradation process. Based on the analysis of the key metabolites, the engineered bacteria were supplemented at 7-day intervals in batches so that each engineered strain maintained its optimal degradation ability. The 21-day degradation ratio finally reached 90.66%, which was much higher than what was observed with simultaneous inoculation. These findings suggest that the three engineered strains with separate modules constructed in this study offer an attractive solution for removing PAHs from the environment.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Junlan Li,Wanli Peng,Xianqi Yin,Xiaozheng Wang,Zhixiang Liu,Qinchen Liu,Zixin Deng,Shuangjun Lin,Rubing Liang
Phenanthrene, a typical chemical of polycyclic aromatic hydrocarbons (PAHs) pollutants, severely threatens health of wild life and human being. Microbial degradation is effective and environment-friendly for PAH removal, while the phenanthrene-degrading mechanism in Gram-positive bacteria is unclear. In this work, one Gram-positive strain of plant growth-promoting rhizobacteria (PGPR), Pseudarthrobacter sp. L1SW, was isolated and identified with high phenanthrene-degrading efficiency and great stress tolerance. It degraded 96.3% of 500 mg/L phenanthrene in 72 h and kept stable degradation performance with heavy metals (65 mg/L of Zn 2+ , 5.56 mg/L of Ni 2+ , and 5.20 mg/L of Cr 3+ ) and surfactant (10 CMC of Tween 80). Strain L1SW degraded phenanthrene mainly through phthalic acid pathway, generating intermediate metabolites including cis -3,4-dihydrophenanthrene-3,4-diol, 1-hydroxy-2-naphthoic acid, and phthalic acid. A novel metabolite ( m/z 419.0939) was successfully separated and identified as an end-product of phenanthrene, suggesting a unique metabolic pathway. With the whole genome sequence alignment and comparative genomic analysis, 19 putative genes associated with phenanthrene metabolism in strain L1SW were identified to be distributed in three gene clusters and induced by phenanthrene and its metabolites. These findings advance the phenanthrene-degrading study in Gram-positive bacteria and promote the practical use of PGPR strains in the bioremediation of PAH-contaminated environments.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Shanshan Sun,Haizhen Wang,Yuanzhi Chen,Jun Lou,Laosheng Wu,Jianming Xu
Mycobacterium sp. WY10 was a highly effective PAHs-degrading bacterium that can degrade phenanthrene (PHE, 100 mg L −1 ) completely within 60 h and 83% of pyrene (PYR, 50 mg L -1 ) in 72 h. In this study, ten and eleven metabolites, respectively, were identified in PHE and PYR degradation cultures, and a detailed PHE and PYR metabolism maps were constructed based on the metabolic results. The strain WY10 degraded PHE and PYR with initial dioxygenation mainly on 3,4- and 4,5-carbon positions, respectively. Thereafter, PYR degradation entered the PHE degradation pathway via the ortho -cleavage. It was observed that the “lower pathway” of PHE and PYR degradations were different. Based on the kinetics of residual metabolites, PHE was degraded in a dominant phthalate pathway and a minor salicylate pathway. However, both phthalate and salicylate pathways played important roles on PYR degradation. The WY10 genome revealed there were fifty-three genes related to PAHs degradations, including a complete gene set for PHE and PYR degradation via the phthalate pathway. The candidate gene/ORF, BOH72_19755, encoding salicylate synthase might contribute in the salicylate pathway.
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JOURNAL OF BACTERIOLOGY
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2017
·Vol. 200
·期 1
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IF 3.143
Hao Yu,Shuxue Zhao,Lizhong Guo
The 1,125-bp mabB gene encoding 5-aminosalicylate (5ASA) 1,2-dioxygenase, a nonheme iron dioxygenase in the bicupin family that catalyzes the cleavage of the 5ASA aromatic ring to form cis-4-amino-6-carboxy-2-oxohexa-3,5-dienoate in the biodegradation of 3-aminobenzoate, was cloned from Comamonas sp. strain QT12 and characterized. The deduced amino acid sequence of the enzyme has low sequence identity with that of other reported ring-cleaving dioxygenases. MabB was heterologously expressed in Escherichia coli cells and purified as a His-tagged enzyme. The optimum pH and temperature for MabB are 8.0 and 10°C, respectively. FeII is required for the catalytic activity of the purified enzyme. The apparent Km and Vmax values of MabB for 5ASA are 52.0 ± 5.6 μM and 850 ± 33.2 U/mg, respectively. The two oxygen atoms incorporated into the product of the MabB-catalyzed reaction are both from the dioxygen molecule. Both 5ASA and gentisate could be converted by MabB; however, the catalytic efficiency of MabB for 5ASA was much higher (∼70-fold) than that for gentisate. The mabB-disrupted mutant lost the ability to grow on 3-aminobenzoate, and mabB expression was higher when strain QT12 was cultivated in the presence of 3-aminobenzoate. Thus, 5ASA is the physiological substrate of MabB.IMPORTANCE For several decades, 5-aminosalicylate (5ASA) has been advocated as the drug mesalazine to treat human inflammatory bowel disease and considered the key intermediate in the xenobiotic degradation of many aromatic organic pollutants. 5ASA biotransformation research will help us elucidate the microbial degradation of these pollutants. Most studies have reported that gentisate 1,2-dioxygenases (GDOs) can convert 5ASA with significantly high activity; however, the catalytic efficiency of these enzymes for gentisate is much higher than that for 5ASA. This study showed that MabB can convert 5ASA to cis-4-amino-6-carboxy-2-oxohexa-3,5-dienoate, incorporating two oxygen atoms from the dioxygen molecule into the product. Unlike GDOs, MabB uses 5ASA instead of gentisate as the primary substrate. mabB is the first reported 5-aminosalicylate 1,2-dioxygenase gene.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Li-Hong Su,Hai-Long Qian,Shu-Ting Xu,Cheng Yang,Xiu-Ping Yan
Specific recognition and selective extraction of mycotoxin in environmental and food matrixes is significant to guarantee public health. Covalent organic frameworks (COFs) are promising adsorbents with tailorable functionality, but their low binding affinity and poor selectivity hamper their wide application for selective extraction of trace mycotoxin from complex matrix. Herein, we report calixarene incorporated molecular imprinting on COF to prepare molecularly imprinted calix[4]arene-containing COF (MICOF-CX4) for supramolecular recognition and specific adsorption of citrinin. Calixarene with host-guest chemistry was used as a functional monomer, while amine units with different topologies and function groups were selected to regulate MICOF-CX4 to match with citrinin. The complementary shape and supramolecular interactions of MICOF-CX4 gave highly selective recognition for citrinin. Moreover, MICOF-CX4 with vast accessible surface and plentiful imprinting sites exhibited faster adsorption kinetics and 4-fold higher adsorption capacity for citrinin adsorption than no-imprinted COF-CX4. Combination of MICOF-CX4 based solid-phase extraction with high-performance liquid chromatography-mass spectrometry allowed interference free determination of trace citrinin in real samples with a low detection limit of 0.03 ng mL −1 , good precision of 4.5 % and quantitative recovery of 88.2 %−101.4 %. The cooperative functions of calixarene and molecular imprinting make COF promising adsorbent for specific adsorption of trace targets in complex matrixes.
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JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Sihui Ding,Yu Xu,Song Xue,Ang Li,Qi Zhang
Capillary electrophoresis (CE) has conventionally been classified into aqueous and non-aqueous categories based on the types of buffer solvents employed. Traditionally, non-aqueous CE has always been associated with the use of organic solvents, which are considered hazardous to health and environmentally detrimental. In this work, we introduce deep eutectic solvents (DESs) as CE separation media for the first time, presenting a novel and environmentally friendly approach to CE separations. The DES employed consists of proline and urea (Proline:Urea, PU), both of which are naturally occurring compounds that are readily available, cost-effective, and environmentally benign. Various fundamental aspects of the DES-type CE media were investigated, including thermal property, viscosity, electroconductivity, Joule heating effect, and compatibility with detectors. A simulated complex mixture of ten naphthalene-based compounds with varied charges and sizes was separated using the DES-based medium in capillary zone electrophoresis (CZE) mode. Moreover, we also established a DES-based micellar electrokinetic chromatography (MEKC) system utilizing Tween-20 as the surfactant. Six structurally similar naphthalene derivatives (isomers) that couldn't be resolved by CZE were effectively separated due to their strong hydrophobic interaction with Tween-20 micelles within the DES medium. Given that DESs are “designer” solvents with highly tunable properties and environmentally friendly characteristics, this study demonstrates the potential of employing DESs as an alternative to organic solvents for greener CE separations.
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EUROPEAN JOURNAL OF PHARMACEUTICS AND BIOPHARMACEUTICS
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2024
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IF 4.4
Xiaoxiao Liang,Shiyuan Liu,Zebin Li,Yuehua Deng,Yanbin Jiang,Huaiyu Yang
Cocrystal engineering, which involves the self-assembly of two or more components into a solid-state supramolecular structure through non-covalent interactions, has emerged as a promising approach to tailor the physicochemical properties of active pharmaceutical ingredient (API). Efficient coformer screening for cocrystal remains a challenge. Herein, a prediction strategy based on machine learning algorithms was employed to predict cocrystal formation and seven reliable models with accuracy over 0.890 were successfully constructed. Imatinib was selected as the model drug and the models established were applied to screen 31 potential coformers. Experimental verification results indicated RF-8 is the optimal model among seven models with an accuracy of 0.839. When the seven models were combined for coformer screening of Imatinib, the combinational model achieved an accuracy of 0.903, and eight new solid forms were observed and characterized. Benefiting from intermolecular interactions, the obtained multicomponent crystals displayed enhanced physicochemical properties. Dissolution and solubility experiments showed the prepared multicomponent crystals had higher cumulative dissolution rate and remarkably improved the solubility of imatinib , and IM-MC exhibited comparable solubility to Imatinib mesylate α form. Stability test and cytotoxicity results showed that multicomponent crystals exhibited excellent stability and the drug-drug cocrystal IM-5F exhibited higher cytotoxicity than pure API.
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TALANTA
·
2024
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IF 5.6
Sihui Ding,Yu Xu,Song Xue,Siyao Liu,Haoxiang Meng,Qi Zhang
β-cyclodextrin (β-CD), as an important pseudo-stationary phase (PSP) in capillary electrophoresis (CE), frequently confronts challenges stemming from its limited water solubility, particularly when high concentrations are required for resolving complex analytes. Traditionally, researchers often resort to the use of (toxic) organic solvents to enhance the solubility of β-CD, establishing non-aqueous capillary electrophoresis (NACE) for specific separations. However, such practices are hazardous to health and run counter to the principles of green analytical chemistry. In this study, we demonstrate a deep eutectic solvent (DES), Proline:Urea (PU), as a promising alternative to conventional organic solvents for β-CD-based CE separations. The DES exhibits a solubility of up to 30% for β-CD, a significant improvement compared to the 1.8% solubility in the aqueous phase. Utilizing this DES-type separation medium, we achieved simultaneous baseline separation of a complex analyte composed of eight structurally similar naphthoic acid derivatives. Furthermore, we conducted a systematic comparison of β-CD's performance in aqueous CE buffers, organic solvents, and DESs, highlighting the superiority of this novel and environmentally friendly CE separation medium.
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Energy & Environmental Science
·
2025
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IF 30.8
Zhongbin Pan,Yu Cheng,Zhicheng Li,Pang Xi,Peng Wang,Xu Fan,Hanxi Chen,Jinjun Liu,Junfei Luo,Jinhong Yu,Minhao Yang,Jiwei Zhai,Weiping Li
Electrostatic capacitors are typically necessary to operate in harsh-temperature environments to fulfill the demanding requirements of renewable energy, electrified transportations, and advanced propulsion systems. However, achieving exceptional capacitive performance in polymer dielectrics at elevated temperatures and electric fields remains a formidable challenge owing to the exponential growth of conduction loss. Herein, we propose a new class of polymer dielectric composites comprising polyetherimide (PEI) incorporated with monodispersed aluminum macrocycle (AOC). The Al-O backbone of AOC creates a ring, where electron-rich O atoms own a strong charge scattering effect and electron-deficient Al atoms have a charge captured capability. Such a unique structure reduces both electron concentration and mobility, thereby effectively inhibiting charge transport within polymer dielectrics and significantly suppressing the high-temperature electrical conduction loss even at high electric fields. Consequently, the PEI-AOC composite exhibits the maximum discharged energy density with an efficiency above 90% of 6.57 J/cm3 and 4.4 J/cm3 at 150°C and 200 °C, which exceed those of the original dielectric by more than ten-fold under identical conditions. This work presents a groundbreaking approach to manipulate the high-temperature capacitive performance of polymer dielectrics in practical power apparatus and electronic devices.
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