ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 412
·期 23
·5653-5661
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IF 3.637
Xie Wei,Zhang Jian,Zeng Yanbo,Wang Hailong,Yang Yiwen,Zhai Yunyun,Miao Dongwei,Li Lei
A novel molecularly imprinted fluorescent sensor for the determination of 4-nitroaniline (4-NA) was synthesized via free radical polymerization with 3-[(7-methoxy-2-oxo-2 H -chromen-4-yl)methyl]-1-vinyl-1 H -imidazol-3-ium bromide as the fluorescence functional monomer, 4-NA as the template molecule, ethylene glycol dimethacrylate as the cross-linker, and 2,2′-azo(bisisobutyronitrile) as the initiator. The obtained fluorescent poly(ionic liquid) was characterized through Fourier transform infrared, scanning electron microscopy, Brunauer–Emmett–Teller analysis, and fluorescence spectrophotometry. The fluorescent sensor had high fluorescence intensity, short detection time (0.5 min), good selectivity, and excellent sensitivity (limit of detection = 0.8 nM) for 4-NA, with good linear relationships of 2.67–10,000 nM. The practical applicability of the fluorescence sensor in detecting 4-NA in industrial wastewater and spiked environmental water was demonstrated, and a satisfactory result was obtained.
Highly sensitive and selective detection of 4-nitroaniline in water by a novel fluorescent sensor based on molecularly imprinted poly(ionic liquid)
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiaojuan Li,Fengzhen Liao,Lanmei Ye,Lizhi Yeh
In this study, based on the extensive discussion of the phase transformation process of metal-organic frameworks (MOFs)——MIL-88A(Fe) under thermal treatment, the catalytic performance of MIL-88A-derived iron/carbon (FexC) composites on persulfate (PS) activation for phenol degradation was investigated. FexC-600 ( γ -Fe 2 O 3 /C) exhibited a superior catalytic activity on PS activation for phenol degradation due to higher carbon content, more sp 2 -hybridized structure, carbonyl group and defective sites in composites, in which 98.23% of phenol (20 mg/L) was degraded after 60 min with 0.3 g/L catalyst and 0.3 g/L PS at ambient pH (6.1). The phenol degradation experiments and mechanism studies revealed that there was a catalytic synergism between iron oxides and carbon component in FexC 400-600 composites. Moreover, sulfate radicals (SO 4 − ), hydroxyl radical (•OH), singlet oxygen ( 1 O 2 ) and interfacial electron transfer process all involved in the degradation of phenol by FexC 400-600 composites, but the 1 O 2 -mediated non-radical oxidation was the dominant pathway rather than reactive radicals. Finally, the possible mechanism of PS activation on FexC 400-600 composites was proposed. This work discusses the synergistic catalytic mechanism of FexC composites on PS activation, and favors to provide a better understanding of the metal species and carbon component interaction in iron/carbon-based materials.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
·
IF 7.864
Wenxiao Zheng,Liuyi Zhu,Sheng Liang,Jinshao Ye,Xin Yang,Zhenchao Lei,Zhang Yan,Yongdong Li,Chaohai Wei,Chunhua Feng
Inorganic constituents in real wastewater, such as halides and carbonates/bicarbonates, may have negative effects on the performance of electrochemical systems because of their capability of quenching HO•. However, we discovered that the presence of Cl– and HCO3– in an electrochemical system is conducive to the formation of ClO•, which plays an important role in promoting the simultaneous elimination of biorefractory organics and nitrogen in secondary coking wastewater effluent. The 6-h operation of the coupled electrochemical system (an undivided electrolytic cell with a PbO2/Ti anode and a Cu/Zn cathode) at a current density of 37.5 mA cm–2 allowed the removal of 87.8% of chemical oxygen demand (COD) and 86.5% of total nitrogen. The electron paramagnetic resonance results suggested the formation of ClO• in the system, and the probe experiments confirmed the predominance of ClO•, whose steady-state concentrations (8.08 × 10–13 M) were 16.4, 26.5, and 1609.5 times those of Cl2•– (4.92 × 10–14 M), HO• (3.05 × 10–14 M), and Cl• (5.02 × 10–16 M), respectively. The rate constant of COD removal and the Faradaic efficiency of anodic oxidation obtained with Cl– and HCO3– was linearly proportional to the natural logarithm of the ClO• concentration, and the specific energy consumption was inversely correlated to it, demonstrating the crucial role of ClO• in pollutant removal.
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CHEMOSPHERE
·
2020
·
IF 5.778
Tianxin Zhu,Jing Deng,Mengyuan Xu,Anhong Cai,Cheng Ye,Jun Li,Xueyan Li,Qiongsong Li
The degradation of N,N -diethyl- meta -toluamide (DEET) in aqueous solution by the UV/monochloramine (UV/NH 2 Cl) process was examined systematically in this study. DEET was resistant to UV photolysis and chloramination, while the synchronous combination of UV irradiation and NH 2 Cl can effectively eliminate DEET, which was caused by the generation of hydroxyl radicals and reactive chlorine species. The former played the critical role in DEET degradation, while the contribution of the latter can be ignored. Under all investigated experimental conditions, DEET degradation in the UV/NH 2 Cl process followed the pseudo-first-order kinetic model. The water quality parameters exerted the complicated impact. Reducing solution pH and raising water temperature both favored the DEET removal. The presence of sulfate, humic acid and fulvic acid accelerated the degradation, while the introduction of bicarbonate and high-concentration chloride retarded the removal. The plausible degradation pathways of DEET in the UV/NH 2 Cl process were proposed through the combination of QTOF/MS analysis and DFT calculation, and mainly involved in the cleavage of C–N bond, dealkylation, mono- and polyhydroxylation. The acute toxicity of reacted solution underwent a trend of first increasing and then decreasing with the prolonged irradiation time, which can be well illustrated by quantitative structure-activity relationship analysis. Electrical energy per order was employed to determine the energy consumption and the optimal conditions were determined as UV fluence of 369.9–493.2 mJ cm −2 and NH 2 Cl dosage of 5–20 mg L −1 .
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Shishu Zhu,Chao Jin,Xiaoguang Duan,Shaobin Wang,Shih-Hsin Ho
Nonradical reactions induced by nanocarbon-driven peroxydisulfate (PDS) activation recently emerge a promising strategy of groundwater remediation or wastewater treatment, whereas the involved reaction pathways remain controversial. We here investigate and differentiate the two representative nonradical mechanisms of PDS activation on graphene-like nanosheets (GNS). The template-induced GNS exhibited a high porosity of over 1200 m 2 g −1 and a few-layered turbostratic structure with graphitic microcrystals. The nonradical oxidation system (aqueous 1 O 2 and nonaqueous electron transfer) of GNS/PDS was highly-reactive, and outperformed graphene- or metal-based activators. Although singlet oxygen ( 1 O 2 ) was detected in the bulk solution, the contribution of 1 O 2 to the entire oxidation were limited (0.004–0.43% and ~6% at neutral and alkaline pH, respectively), determined by chemical probes and steady-state kinetics. Different to the reference product (benzoquinone) of phenol oxidation by photosensitive singlet oxygenation, intermediate product in GNS/PDS was benzoic acid which barely resulted from 1 O 2 oxidation. Furthermore, surface-confined electron transfer was the major oxidation pathway verified by electronic measurement. Surface adsorption rather than hydrophobic effect of organic substrates on GNS accelerated a two-electron transfer. The nonradical oxidation exhibited a dissociation constant ( p Ka)-dependent mechanism because of competitive adsorption with S 2 O 8 2− anions. The findings facilitate a thorough understanding of carbon-catalyzed persulfate activation during in situ chemical oxidation (ISCO) and provide novel insights for the selective removal of aqueous organic contaminants in a nonradical manner.
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WATER RESEARCH
·
2020
·
IF 9.13
Shiqing Zhou,Ling Li,Yangtao Wu,Shumin Zhu,Ningyuan Zhu,Lingjun Bu,Dionysios D. Dionysiou
The presence of nitrite (NO 2 − ) is inevitable with concentrations of several mg L −1 in some typical water bodies. In this study, UV at wavelength of 365 nm was investigated to degrade contaminants of emerging concern (CECs) in the presence of NO 2 − at environmentally relevant concentrations (0.1–5.0 mg L −1 ). Six selected CECs with different structures were efficiently removed because of the generation of reactive nitrogen species (RNS) and hydroxyl radical (HO • ) from photolysis of NO 2 − . Contributions of UV 365 photolysis, RNS, and HO • to CEC degradation in UV 365 /NO 2 − system were calculated, and RNS were found to be the predominant species that are responsible for CEC degradation. The second major contributor is HO • for the degradation of selected CECs except for the case of sulfadiazine. Impacts of water matrix components (including dissolved oxygen, solution pH, and natural organic matter) on CEC degradation in UV 365 /NO 2 − system were evaluated. Furthermore, evolution profiles of CECs and NO 2 − in UV 365 /NO 2 − system were tracked when actual water samples were used as background, and a simultaneous removal of CECs and NO 2 − was observed. Transformation products of bisphenol A and carbamazepine were proposed according to the results of HPLC/MS and quantum chemistry calculations. Nitration induced by RNS and hydroxylation induced by HO • are main reactions occurred during CEC degradation in UV 365 /NO 2 − system. Overall, UV 365 is a potential technology to remove CECs and NO 2 − in aquatic environment when residual NO 2 − is present. Our present study also provides possibility for the application of sunlight to remediate water co-polluted by CECs and NO 2 − .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yue Yin,Mengqi Shi,Yi Ren,Shu Wang,Ming Hua,Junhe Lu,Weiming Zhang,Lu Lv
A novel multifunctional metal-organic frameworks (MOFs) UiO-66@Fe 3 O 4 @UiO-66 (UiO = University of Oslo) was fabricated to adsorb pharmaceuticals and personal care products (PPCPs) under near neutral conditions. We designed a wrinkle structure on the surface of UiO-66@Fe 3 O 4 @UiO-66 by seeded growth strategy. These wrinkles were composed of Fe 3 O 4 nanoparticles and outermost UiO-66. It made the specific surface area of the MOFs increases, and provided multiple active sites for a representative pollutant salicylic acid (SA) adsorption. Moreover, lattice defects formed during secondary growth facilitating the coordination interaction between SA and the secondary building unit of UiO-66@Fe 3 O 4 @UiO-66 under near neutral conditions. These advantages made the adsorption capacity of per unit mass UiO-66 in UiO-66@Fe 3 O 4 @UiO-66 about 42% higher than that of the pristine UiO-66, and the removal rate of 1 mg L −1 SA reach 64.5% in real wastewater. Furthermore, magnetic Fe 3 O 4 particles in the wrinkles exhibited outstanding magnetic separation performance. So that UiO-66@Fe 3 O 4 @UiO-66 can be effectively separated from the liquid media and regenerated after adsorption. The results show that the wrinkled MOFs could be used as an excellent candidate for SA adsorption in real wastewater. More importantly, this strategy could guide the preparation of different kind of MOFs to adsorb PPCPs in wastewater.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 5
·1518-1528
·
IF 5.721
Jin Zhang,Linjuan Pei,Jie Wang,Pengqi Zhu,Xianmo Gu,Zhanfeng Zheng
Ru/TiO2 catalysts exhibit excellent catalytic performance for selective reduction of 4-nitroacetophenone to 4-aminoacetophenone at normal temperature and atmospheric hydrogen pressure. Moreover, 99.9% selectivity to 4-aminoacetophenone can be obtained over 2.7 wt% Ru/TiO2(anatase) catalyst even in a relatively wide temperature (55–115 °C) and time (1–12 h) range. Its excellent catalytic performance is derived from the activation of H2 on the Ru nanoparticles at atmospheric pressure and the strong interaction of nitro groups with the support surface. Additionally, Ru nanoparticles supported on different crystalline TiO2 phases (anatase and rutile) result in different reaction pathways for 4-nitroacetophenone. Since the Ti–Ti distance on the rutile surface is smaller than that on the anatase surface, the hydroxylamine species adsorbed on the Ti atoms of rutile are more susceptible to the coupling reaction. Therefore, Ru/TiO2(rutile) causes a series of intermediates to accumulate during the conversion process, while Ru/TiO2(anatase) allows the highly selective conversion of 4-nitroacetophenone to 4-aminophenone. In addition, Ru/TiO2(anatase) can achieve chemoselective reduction of nitroaromatics to the corresponding anilines in the presence of –CN, –CHO, and –COOH, especially nitroaromatics containing CC and CC, indicating the excellent applicability.
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LUMINESCENCE
·
2021
·Vol. 36
·期 7
·1767-1774
·
IF 2.464
Bing Jie Jia,Min Lin,Jian Ping Wang,Ning Peng Wu
In this study, nitrobenzene was used as dummy template to synthesize a type of specific molecularly imprinted microspheres for chloramphenicol, and 4-nitroaniline was coupled with three fluorophores to synthesize three fluorescent tracers. Then a competitive fluorescence method was developed on a conventional microplate for detection of chloramphenicol in chicken and pork samples. This method contained only one sample-loading step, so one assay was finished within 30 min. The IC 50 was 1.8 ng/ml, and the limit of detection was 0.06 ng/g. The recoveries from chloramphenicol-fortified blank meat samples were in the range 67.5–96.2%. Furthermore, this method could be recycled three times. The detection results for some real meat samples were identical to that of a LC–MS/MS method. Therefore, this method could be used as a practical tool for routine screening for the residue of chloramphenicol in large number of meat samples.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Jing Song,Yongjin Cui,Lin Sheng,Yujun Wang,Chencan Du,Jian Deng,Guangsheng Luo
The kinetics of p -nitrotoluene nitration with mixed acid is important to industrial process design and safety control. However, it's difficult to acquire accurate kinetic data and no kinetics study has ever been reported before because of fast, highly exothermic and heterogeneous characteristics. In this work, a continuous-flow microreactor system including a micromixer, a capillary reactor and an online quenching module was designed to carry out the nitration under a homogeneous reaction condition. The homogeneous nitration can completely eliminate mass transfer resistance between phases, and accurately control reaction temperature and residence time in the continuous-flow microreactor system. The observed reaction rate constants separately based on HNO 3 and NO 2 + , pre-exponential factor and activation energy of p -nitrotoluene nitration were obtained and a general method was established to collect kinetics data for such a kind of fast and highly exothermal nitration reactions.
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ACS ES&T Engineering
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2021
·
IF 0
Zihao Zhao,Xinhong Li,Hongchao Li,Jieshu Qian,Bingcai Pan
The combination of Co(II) and peracetic acid (PAA) is an important alternative advanced oxidation process (AOPs), in which R-O• radicals including acetyloxyl radicals (CH3C(O)O•) and acetylperoxyl radicals (CH3C(O)OO•) have been considered to be the primary reactive species for the oxidative degradation of contaminants. However, it is still unclear how the active Co species participates in this process. In this study, we conduct a series of experiments including chemical probing, radical quenching, electron paramagnetic resonance (EPR), and Co(III) oxidation to investigate the degradation mechanism of contaminants in the Co(II)/PAA process, using bisphenol A (BPA) as target pollutant. On the basis of these results, we propose a Co(II)-PAA complex (Co(II)-OO(O)CCH3) to be the primary reactive species, while R-O• radicals and Co(III) (available as dimeric Co-peroxide species) derived from the decomposition of Co(II)-PAA complex are the minor contributors for the oxidation of BPA. Factors, including PAA concentration, Co(II) concentration, solution pH, inorganic anions, and natural organic matters (NOM), that might affect the oxidation performance of the Co(II)/PAA process were also investigated systematically. This study sheds new light on the mechanistic understanding of the Co(II)/PAA process for the oxidation of contaminants in water.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shizong Wang,Lejin Xu,Jianlong Wang
Metal-free carbonaceous persulfate activator has received increasing attention recently. Graphitic carbon nitride (g-C 3 N 4 ) is one of the promising carbon materials due to excellent stability and low cost, but its activity for peroxymonosulfate (PMS) activation is low. In this study, g-C 3 N 4 was modified with oxygen atoms in the first step (O-g-C 3 N 4 ), then exfoliated via sequential thermal and ultrasound treatment to produce O-g-C 3 N 4 nanoflakes to increase its catalytic activity to activate PMS. In the presence of O-g-C 3 N 4 nanoflakes, SMX degradation rate achieved 0.079 min −1 , which was much faster than that in the presence of pristine g-C 3 N 4 (0.0083 min −1 ) and untreated O-g-C 3 N 4 (0.012 min −1 ). The surface-bound radicals and direct electron transfer between SMX and PMS contributed to the SMX degradation. Density functional theory (DFT) simulation revealed that oxygen-doping changed the charge distribution. Furthermore, O-g-C 3 N 4 nanoflakes had higher adsorption energy for PMS and SMX (0.518 kcal/mol) than pristine g-C 3 N 4 (0.304 kcal/mol), which contributed to the enhanced PMS activation and SMX degradation. Cycling experiments and comparison of characterization results before and after experiments proved that O-g-C 3 N 4 nanoflakes had superior catalytic and structural stability. This study could provide a high efficient metal-free carbonaceous activator of PMS for the degradation of antibiotics in the wastewater.
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