CHEMICAL PAPERS
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2023
·Vol. 77
·期 6
·2967-2976
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IF 2.2
Ma Mingming,Liang Juanli
The voltammetric behavior of 2-aminoazotoluene (2-AMAT) is studied at pencil electrode (PEC) modified by electropolymerization of β-cyclodextrin (P-β-CD-PEC) in different supporting electrolyte at various pH values using cyclic voltammetry (CV) and differential pulse voltammetry (DPV). At the scan rate of 0.1 V s −1 , 2-AMAT exhibits an irreversible oxidation peak at 0.67 V in phosphate buffer solution (PBS) with the pH value of 6.64. The electrochemical data suggest that the oxidation reaction of 2-AMAT at the surface of P−β−CD−PEC involves one electron and one proton. 2−AMAT has a significantly higher oxidation peak current on P−β−CD−PEC than pristine PEC, which is ascribed to the presence of cavities in polymer of β−CD on the surface of PEC. Under the optimized DPV conditions, the oxidation peak current is linear with 2-AMAT concentration in the range of 0.3 μM to 30.0 μM with a low limit of detection (LOD = 0.14 μM) and high sensitivity (1.45 μA /μM). The same 2-AMAT concentration was measured every two days in 20 days using the same P−β−CD−PEC. The results show that the relative standard deviation (RSD) of the peak current was 3.36%, indicating that the stability of P−β−CD−PEC is good. Five different bitches P−β−CD−PEC was used to determine the same 2-AMAT concentration and 4.29% RSD is obtained, which suggests that the reproducibility of this modified electrode is excellent. In addition to some metal ions, the structural substances such as 2,4-diaminotoluene and 4-chloroaniline do not interfere the determination of 2-AMAT, suggesting that P−β−CD−PEC has fine selectivity. Therefore, a new method for detecting 2-AMAT based on P−β−CD−PEC is developed. This method is successfully used to determine 2−AMAT in rose lotion cosmetics with satisfied results.
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JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Ruijuan Duan,Meiling Qi
This work presents the investigation of two new pentiptycene (PP)-functionalized triblock copolymers (PEPE1, PEPE2) for gas chromatographic (GC) analyses with an aim to address the separation problems toward analytes of high resemblance in properties and a wide variety of components in complex samples. Up to date, these two materials are not reported in any fields. The PEPE1 and PEPE2 columns showed close column efficiency (above 4000 plates/m) but differed in polarity, morphology and separation performance. As testified by the challenging Grob test mixture, the PEPE1 column exhibited comprehensively higher separation capability than the PEPE2 column and the commercial reference columns. Also, the PEPE1 column achieved high-resolution performance for both apolar and polar isomers of high resemblance, such as xylenes, phenols and anilines. Moreover, it displayed high inertness towards carboxylic acids and excellent separation repeatability and reproducibility tested by the aniline isomers with the RSD values in the range of 0.01–0.04% for run-to-run, 0.09–0.13% for day-to-day and 1.2–2.0% for column-to-column, respectively. Its application to GC–MS analysis of the essential oil from tea flowers demonstrated its advantageous separation performance towards a wide range of components and proved its feasibility for practical analyses of complex samples.
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JOURNAL OF POWER SOURCES
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2022
·
IF 9.794
Yiming Xiao,Qixuan Ma,Xiaoyu Shen,Songbo Wang,Jun Xiang,Lei Zhang,Penggao Cheng,Xinjun Du,Zhen Yin,Na Tang
Phosphoric acid (PA) doped polybenzimidazole (PBI) membrane has been regarded as one of most effective high temperature proton exchange membrane (HT-PEM). However, it has to face poor mechanical properties at high acid doping levels (ADLs) and significant acid loss at high temperature during the operation of fuel cell. Herein, we prepare cross-linked PBI membranes containing different contents of the cross-linker three-dimensional polyaniline (PANI) via a facile N-substitution reaction. The obtained cross-linked PBI membrane exhibits superior tensile strength , stability and proton conductivity . More importantly, robust mechanical strength and good acid retention of the PA-doped cross-linked PBI membrane are demonstrated even at high ADL (above 20). The cross-linked PANI-30%-g-OPBI membrane exhibits a high ADL of 22.9, high proton conductivity of 122.8 mS cm −1 at 160 °C. Furthermore, the peak power density reaches 447 mW cm −2 at 160 °C, which is 2.5 times than that based on the corresponding PBI membrane. Molecular dynamics simulation results indicate that the decreased mobility of polymer chains improve the mechanical properties of the cross-linked membranes, and the high intermolecular interaction energy of the aniline-biphosphate ion pair significantly decrease PA leaching in the membranes due to the introduction of 3D molecular structure of PANI.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Hao Wang,Hui Yun,Xiaodan Ma,Minghan Li,Mengyuan Qi,Ling Wang,Zhiling Li,Shuhong Gao,Yu Tao,Bin Liang,Aijie Wang
Chlorinated antimicrobial triclocarban (3,4,4′-trichlorocarbanilide, TCC) is an emerging refractory contaminant omnipresent in various environments. Preferential microbial hydrolysis of TCC to chloroanilines is essential for its efficient mineralization. However, the microbial mineralization of TCC in domestic wastewater is poorly understood. Here, the bioelectrochemical catabolism of TCC to chloroanilines (3,4-dichloroaniline and 4-chloroaniline) and then to CO 2 was realized through the cascade acclimation of TCC-hydrolyzing and chloroanilines-oxidizing microbial communities . The biodegradation of chloroanilines was obviously enhanced in the bioelectrochemical reactors. Pseudomonas , Diaphorobacter , and Sphingomonas were the enriched TCC or chloroanilines degraders in the bioelectrochemical reactors. The addition of TCC enhanced the synergistic effect within functional microbial communities based on the feature of the phylogenetic ecological networks. This study provides a new idea for the targeted domestication and construction of functionally differentiated microbial communities to efficiently remove TCC from domestic wastewater through a green and low-carbon bioelectrochemical method.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Di Zhang,Tom Bond,Yang Pan,Mingli Li,Jiayi Luo,Rong Xiao,Wenhai Chu
Identifying disinfection byproducts (DBPs) with high health risk is an unresolved challenge. In this study, six members of a new class of aromatic nitrogenous DBPs─2-chloroaniline, 2-bromoaniline, 2,4-dichloroaniline, 2-chloro-4-bromoaniline, 4-chloro-3-nitroaniline, and 2-chloro-4-nitroaniline─are reported as DBPs in drinking water for the first time. Haloanilines completely degraded within 1 h in the presence of chlorine (1 mg/L), while about 20% remained in the presence of chloramine (1 mg/L) after 120 h. Haloanilines showed high stability in the absence of disinfectants, with <30% degradation at pH 5–9 over 120 h. Eight haloanilines were determined in chloraminated finished water and tap water at total concentrations of up to 443 ng/L. The most abundant was 2-bromoaniline, with a median concentration of 104 ng/L. The cytotoxicity of eight haloanilines and regulated trichloromethane and dichloroacetic acid (DCAA) was evaluated using Hep G2 cell assay. The EC50 values of eight haloanilines were 1–2 orders of magnitude lower than those of the regulated DBPs. The lowest toxic concentration of 2-chloro-4-nitroaniline was 1 μM, 500 times lower than that of DCAA. The formation and control of haloanilines in drinking water warrant further investigation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Chunyan Li,Yueling Sun,Guanjun Sun,Hailian Zang,Shanshan Sun,Xinyue Zhao,Ning Hou,Dapeng Li
Triclocarban (TCC) is an emerging and intractable environmental contaminant due to its hydrophobicity and chemical stability. However, the antibacterial property of TCC limits its biodegradation, and only the functional enzyme TccA involved in TCC degradation has been characterized to date. In this study, we report a highly efficient TCC-degrading bacterium, Rhodococcus rhodochrous BX2, that could degrade and mineralize TCC (10 mg/L) by 76.8% and 56.5%, respectively, within 5 days. Subsequently, the TCC biodegradation pathway was predicted based on the detection of metabolites using modern mass spectrometry techniques. Furthermore, an amidase (TccS) and a novel phenol hydroxylase (PH IND ) encoded by the tccS and PH IND genes, respectively, were identified by genomic and transcriptomic analyses of strain BX2, and these enzymes were further unequivocally proven to be the key enzymes responsible for the metabolism of TCC and its intermediate 4-chloroaniline (4-CA) by using a combination of heterologous expression and gene knockout. Our results shed new light on the mechanism of TCC biodegradation and better utilization of microbes to remediate TCC contamination.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Cholnam Ri,Fengxiang Li,Hyokchol Mun,Linan Liu,Jingchun Tang
The technology of integrating sulfidated zero-valent iron and functional anaerobic bacteria has been extensively explored to improve the removal efficiency of pollutants and enhance the performance of anaerobic microbial system. In this study, the simultaneous DCNB(2,4-dichloronitrobenzene) reduction and methane production by ball-milled 1:1 Fe 0 /FeS 2 (briefly, 1:1 Fe 0 /FeS 2 ), Shewanella oneidensis MR-1 and microbial consortium (MC) were firstly investigated. The result showed that the DCNB reduction was increased by 2.6 and 1.7 times in 1:1 Fe 0 /FeS 2 + MR-1 group compared to 1:1 Fe 0 /FeS 2 and MR-1, respectively, while it further increased by almost 2 times in 1:1 Fe 0 /FeS 2 + MC + MR-1 group as compared to that of 1:1 Fe 0 /FeS 2 + MR-1 group. Moreover, the methane production was drastically facilitated via the reciprocal interaction among FeS as the reaction product, MR-1 and MC. Dechlorination was not found, mainly due to the inability of 1:1 Fe 0 /FeS 2 and the inexistence of dechlorinating bacteria in original inoculum. Meanwhile, the microbial community was also changed, with genera like Eubacterium capable of reducing nitroaromatic compound and Methanosarcina as acetoclastic methanogen enriched by 1:1 Fe 0 /FeS 2 and MR-1. Therefore, fast DCNB reduction and methane production using 1:1 Fe 0 /FeS 2 in anaerobic microbial system, gives useful reference for both establishment of pollutant removal and biogas production. In conclusion, Fe 0 /FeS 2 , as a kind of sulfidated ZVI, is a good candidate for enhancing both pollutant degradation and CH 4 production in anaerobic wastewater treatment.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Zhe,Wang Chunpeng,Mao Shanjun,Lu Bing,Chen Yuzhuo,Zhang Xie,Chen Zhirong,Wang Yong
Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here, a novel orthogonal decomposition method is firstly proposed to settle this issue in p -chloronitrobenzene hydrogenation reaction on size- and shape-controlled Pt nanoparticles (NPs) carried on various supports. Results suggest Fermi levels of catalysts can be modulated by supports with varied work function ( W f ). And the selectivity on Pt NPs of similar size and shape is linearly related with the W f of support. Optimized Fermi levels of the catalysts with large W f weaken the ability of Pt NPs to fill valence electrons into the antibonding orbital of C–Cl bond, finally suppressing the hydrodehalogenation side reaction. Foremost, the geometric effect is firstly spun off through orthogonal relation based on series of linear relationships over various sizes of Pt NPs reflecting the electronic effect. Moreover, separable nested double coordinate system is established to quantitatively evaluate the two effects.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Zhuang Ke,Shen Wang,Wenqi Zhu,Fu Zhang,Wenjing Qiao,Jiandong Jiang,Kai Chen
Triclocarban, one of the emerging pollutants, has been accumulating, and it is frequently detected in wastewater. Due to its toxicity and persistence, the efficient removal of triclocarban from wastewater systems is challenging. Genetic bioaugmentation with transferable catabolic plasmids has been considered to be a long-lasting method to clean up pollutants in continuous flow wastewater treatment systems. In this study, bioaugmentation with Pseudomonas putida KT2440, harboring the transferrable triclocarban-catabolic plasmid pDCA-1- gfp-tccA2 , rapidly converted 50 μM triclocarban in wastewater into 3,4-dichloroaniline and 4-chloroaniline, which are further mineralized more easily. RT-qPCR results showed that the ratio of the copy number of pDCA-1- gfp-tccA2 to the cell number of strain KT2440 gradually increased during genetic bioaugmentation, suggesting horizontal transfer and proliferation of the plasmid. By using DNA stable isotope probing (SIP) and amplicon sequencing, OTU86 ( Escherichia - Shigella ), OTU155 ( Citrobacter ), OTU5 ( Brucella ), and OTU15 (Enterobacteriaceae) were found to be the potential recipients of the plasmid pDCA-1- gfp-tccA2 in the wastewater bacterial community. Furthermore, three transconjugants in the genera of Escherichia , Citrobacter , and Brucella showing triclocarban-degrading abilities were isolated from the wastewater. This study develops a new method for removing triclocarban from wastewater and provides insights into the environmental behavior of transferrable catabolic plasmids in bacterial community in wastewater systems.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Hao Wang,Hui Yun,Minghan Li,Hanlin Cui,Xiaodan Ma,Yanqing Zhang,Xuanyuan Pei,Liying Zhang,Ke Shi,Zhiling Li,Bin Liang,Aijie Wang,Jizhong Zhou
Triclocarban (TCC), one of the typical antimicrobial agents, is a contaminant of emerging concern commonly found in high concentration in water environments. However, the fate and toxicity of TCC in wastewater treatment systems remain poorly understood. Here, we investigated how TCC impacts chemical oxygen demand and inorganic nitrogen transformation in a hydrolytic anaerobic-anoxic/oxic process. In the anaerobic section, the transformation of TCC was dominated by reductive dechlorination and supplemented by two amid bonds hydrolysis. In the anoxic and oxic sections, the hydrolysis of amid bonds dominated. The toxicity was reduced after the treatment (IC 50 from 0.09 to 0.54). TCC inhibited NH 4 + -N removal in the anaerobic section and led to the NO 3 - -N accumulation (2.84–4.13 mg/L) after treatment, with the abundance of N-removal bacteria decreased by 6%. Furthermore, the original ecological niche was gradually replaced by TCC-resistant/degradative bacteria, formating new microbial modules to resist the TCC stress. Importantly, fourteen genera including Methanosaeta , Longilinea , Dokdonella and Mycobacterium as potential bioindicators warning TCC and its intermediates were proposed. Overall, this study provides new insights into the fate of TCC in biological wastewater treatment systems and suggests a great importance for TCC control to ensure the health and resilience of ecosystems.
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ACS ES&T Engineering
·
2021
·
IF 0
Ying Liu,Yulin Yang,Wei Miao,Ningjie Du,Dandan Wang,Hehe Qin,Shun Mao,Kostya Ken Ostrikov
Electro-Fenton (EF) is one of the promising clean and renewable technologies for organic pollutant control. However, insufficient hydrogen peroxide (H2O2) generation and the subsequent hydroxyl radicals (•OH) conversion still prevent the wide applications of EF. Herein, we report a Ce-doped vertically aligned α-FeOOH nanoflakes anchored on a carbon felt (CF) cathode for EF operation. In this system, a high concentration H2O2 (113.6 mg/L on 4 cm2 cathode) is generated in 60 min, and being efficiently catalyzed to •OH by virtue of the active nanoedge (1.6 nm thickness) of Ce-doped α-FeOOH. The •OH production rate is calculated as high as 4.2 mM/W/cm2/min, which is ∼6.6-fold higher compared with the unmodified CF electrode. Moreover, this novel cathode achieves a complete removal (100% removal rate) of ultrahigh concentration chloramphenicol (1.1 mM, 355 mg/L) in 8 h and a high mineralization rate (94%) in 29 h in a scaled-up EF system. Density functional theory calculations (DFT) reveal that the Ce doping in α-FeOOH greatly promotes the conversion of H2O2 into •OH. This study not only offers a novel cathode structure for EF process but also opens radically new prospects for applied environmental catalysis.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2021
·
IF 5.279
Shouchun Xiao,Shengchen Lv,Zheng Cheng,Caiwei Hu,Pengxi Li,Fang Nan,Xueke Liu,Donghui Liu,Zhiqiang Zhou,Peng Wang
A simple and effective pretreatment method based on matrix solid-phase dispersion was developed for the determination of pharmaceutical and personal care products (PPCPs) and their metabolites in fish by high-performance liquid chromatography tandem mass spectrometry. The type and amount of dispersant, adsorbent, and eluting solvent were optimized by a single-factor experiment and Box–Behnken design. Under the optimal conditions with 2.5 g of Florisil as a dispersant, 500 mg of C18 as an adsorbent, and 5 mL of acetonitrile as an eluting solvent, the recoveries ranged from 70.4 to 99.9% with relative standard deviations less than 10.5%, and the limits of quantitation ranged from 0.13 to 1.01 μg/kg. The developed method was successfully applied to detect PPCPs in marketed fish, and five PPCPs, including triclocarban, sulfadiazine, sulfadimidine, sulfamethoxazole, and carbamazepine, were detected at trace levels. The proposed method, which has the advantages of short analysis time, less solvent consumption, and high sensitivity, can be used for the determination of trace PPCPs in fish.
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