ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Muhammad Saqib,Shahida Bashir,Haijuan Li,ShanShan Wang,Yongdong Jin
Development of simple and effective chemiluminescence (CL) systems for multiple sensing applications is significantly important but still a challenge. Until now, the majority of CL systems primarily utilized hydrogen peroxide (H2O2) as coreactant, which is limited in its stability and selectivity due to the easy decomposition of H2O2 in the presence of several ions. In this study, we develop a new and intense CL system by combined use of tris(2-carboxyethyl)phosphine (TCEP), a highly solution stable and pH-tolerant tertiary phosphine, with lucigenin for the first time. The effective pairing leads to a significant ∼23 times CL enhancement over classic the lucigenin–H2O2 system without employing additional catalysts. By virtue of this fascinating platform, a sensitive CL method has been developed for the multiple detection of TCEP (LOD = 70 nM), lucigenin (LOD = 4.0 nM), superoxide dismutase (LOD = 0.8 ng/mL), Hg2+(LOD = 0.3 nM), and dopamine (LOD = 3.0 nM), with a linear range of 0.1–320 μM, 0.01–55 μM, 0.005–0.5 μg/mL, 1.0–600 nM, and 0.01–0.8 μM, respectively. Remarkably, this CL method exhibited superior selectivity over several potential interferents. Moreover, the proposed method achieved excellent recoveries in the range of 94.0–102.3% for both Hg2+ detection in lake water and dopamine detection in human serum real samples. We envision that broad applications of TCEP may lead to construct new CL systems, pushing forward for efficient detection of various analytes.
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高影响因子
WATER RESEARCH
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2018
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IF 7.051
Da Wang,Haodan Xu,Jun Ma,Stefanos Giannakis,Xiaohui Lu,Huizhong Chi,Shuang Song,Jingyao Qi
A light-weight granular mixed-quartz sand (denoted as L-GQS) combined with stirring-assisted bubble column reactor was firstly applied in catalytic ozonation of atrazine. The L-GQS, with a density of 2.36 g cm −3 and average diameter of ca. of 4 mm, was readily churned up and uniformly distributed within the solution in the reactor. The introduction of L-GQS was found to exhibit enhanced catalytic ozonation of atrazine, with the increase in degradation rate and the dissolved organic carbon (DOC) removal being more than 2-fold for the catalytic process (L-GQS dosage = 5 g L −1 , [atrazine] 0 = 50 μM, [O 3 ] = 25 mg L −1 , gas flow = 0.2 L min −1 , at pH 7.0 and 293 K). The L-GQS settled at the bottom of the reactor after experimentation, allowing its easy separation from the solution. A complete characterization of the material (XRD, XPS, FTIR , FE-SEM/EDS, BET and pH pzc ) revealed that L-GQS consisted of α-quartz, β-cristobalite, anorthoclase and small amount of iron oxy-hydroxides. Hydroxyl groups, Bronsted acid sites and Lewis acid sites on the surface of L-GQS all contributed to the atrazine adsorption, ozone decomposition and ·OH generation. The L-GQS catalyzed ozonation exhibited superior atrazine degradation and mineralization rates in a wide range of pH (3.0–9.0) and reaction temperatures (278 K–293 K). Also, an enhancement of DOC abatement was observed both in presence of natural organic matter isolates and natural water matrices (river water) when L-GQS was used. Finally, the degradation mechanism was proposed, based on the intermediates and by-products formation analyzed by LC-QTOF-MS/MS and ionic chromatography. Our results indicate that the L-GQS combined with stirring-assisted bubble column reactor could be utilized as an enhancement of ozone-based advanced oxidation processes .
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NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 24
·19571-19577
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IF 3.201
Jingyu Sun,Haiming Xu,Dongya Li,Zhongwei Zou,Qiyuan Wu,Guoguan Liu,Jia Yang,Lei Sun,Dongsheng Xia
A feathery-shaped form of BiOCl (BOC-M) with a high concentration of oxygen vacancies was successfully synthesized using the ultrasound method at room temperature with maltitol as a surfactant. BOC-M was found to exhibit excellent visible-light photocatalytic activities for the degradations of the antibiotic tetracycline hydrochloride (TC-HCl) and rhodamine B (RhB), whose reaction rate was found to be approximately 3 times higher than that using bulk BiOCl (BOC). The enhanced visible photocatalytic performance of BOC-M was ascribed to its high concentration of oxygen vacancies, large specific surface area and strong hydrophilicity. Moreover, the photocatalytic reaction mechanism was further revealed by performing radical- and hole-trapping experiments and electron spin resonance spectroscopy (ESR). The results suggested that ˙O2− was the main active species during the degradation process. This work provided a facile and scalable method to synthesize maltitol-assisted Bi-based photocatalysts and shed light on the highly efficient catalysis offered by BiOCl resulting from the oxygen vacancies produced by the new synthetic route we developed.
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Journal of the Taiwan Institute of Chemical Engineers
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2018
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IF 3.849
Chunxue Li,Huinan Che,Chunbo Liu,Guangbo Che,Paul. A. Charpentier,William Z. Xu,Xiuyan Wang,Lihui Liu
In this study, we report a facile and green strategy to produce graphitic carbon nitride quantum dots (g-C 3 N 4 QDs)/BiVO 4 Z-scheme nanoheterostructure, which is composed by g-C 3 N 4 QDs assembled on the surface of mesh-like BiVO 4 crystals. As compared with pure BiVO 4 , the g-C 3 N 4 QDs/BiVO 4 composite showed significantly enhanced photocatalytic performance towards degradation of rhodamine B (RhB) and Tetracycline (TC) under visible light irradiation, which is attributed to the increased surface area, (increased number of photocatalytically active sites) and the improved efficiency of separation of photogenerated electron-hole pairs through an efficient charge transfer Z-scheme system. The stability and durability of photocatalyst are also discussed in detail. Moreover, the possible enhanced photocatalytic mechanism was put forwarded and explained by the electron spin resonance (ESR) spin-trap technique and active species trapping experiments. The successful implementation of this work will have guiding significance for the preparation of photocatalysts, and provide theoretical basis and experimental guidance for future development of Z-scheme photocatalytic mechanism of the hybrid photocatalysts with better performance.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yanan Shang,Cheng Chen,Ping Zhang,Qinyan Yue,Yanwei Li,Baoyu Gao,Xing Xu
In this work, the nitrogen-doped carbon nanotubes with encapsulated Fe 3 C nanoparticles (Fe 3 C@NCNTs) were prepared through a simple process by pyrolyzing the precursor of ferric trichloride hexahydrate and melamine composite. It was studied systematically that multiple Fe 3 C@NCNTs synthesized under 600–1000 °C activated persulfate (PS) for the degradation of sulfamethoxazole (SMX), a widely used antibiotic of sulfonamides. Raman spectrum , X-Ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS) were used to characterize the transformation of catalyst with the increase of annulling temperature. The Fe 3 C@NCNTs synthesized under 800, 900 and 1000 °C showed similar degradation ability to SMX with degradation rates of 0.650–0.893 min −1 . During catalytic process, the specific structure of Fe 3 C encapsulated NCNTs could both benefit the electron transfer and prevent the Fe 3 C dissolving in the solution. The results of quenching experiments coupling with electron paramagnetic resonance (EPR) spectra suggested the OH, SO 4 − and 1 O 2 contributed to the degradation of SMX and the singlet oxygen took effect for longer time. The degradation intermediates were mainly derived from the reactions of hydroxylation, oxidation , aniline ring opening, deamination, desulfonation, as well as bond cleavage. In terms of the density functional theory (DFT) calculations, the graphitic N exhibited the highest ΔE ads (−0.437 eV) for the PS molecule, and it was followed by the pyrrolic N (−0.304 eV), pristine graphene (−0.146 eV) and pyridine N (−0.072 eV), which means that the graphitic N is more favorable for the binding affinity with PS, forming the reactive complexes on the surface of the NCNTs catalysts to promote the nonradical oxidation.
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CHEMOSPHERE
·
2019
·
IF 5.108
Zhendong Li,Dongfang Liu,Yingxin Zhao,Songrong Li,Xiaocheng Wei,Fansheng Meng,Wenli Huang,Zhongfang Lei
In this study, CuO-CeO 2 was synthesized via an easy hydrothermal-calcination method and innovatively applied to peroxymonosulfate (PMS) activation for pollutants degradation under a non-radical oxidation pathway. Singlet oxygen ( 1 O 2 ) was the dominated reactive oxygen species in the CuO-CeO 2 /PMS system, leading to a dramatical degradation efficiency with Rhodamine B (RhB) as model compounds. The observed rate constant of the CuO-CeO 2 /PMS system was 7–11 times higher than that of only PMS , CeO 2 /PMS and CuO/PMS systems. Also, under the reaction conditions of 1.6 mM PMS, 0.4 g/L catalyst and initial pH 7, the degradation efficiencies of RhB, Methylene Blue , Reactive Blue 19 and atrazine were respectively up to 100%, 85.39%, 72.84% and 98.44% in 60 min. X-ray photoelectron microscopy analysis indicated that the electrons transfer between CuO and CeO 2 and the formation of oxygen vacancy in CeO 2 should be responsible for the enhanced 1 O 2 production, which involved a new non-radical oxidation pathway for PMS activation by CuO-CeO 2 catalyst. Moreover, the combination of CuO and CeO 2 increased reusability and stability of catalyst, allowing it remove more than 92% of RhB over a wide pH range (pH = 3–9). This study not only proved that CuO-CeO 2 is an efficient and stable PMS activator but also provided a new insight into PMS activation through a non-radical oxidation pathway for organic contaminants removal from wastewater.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Nan Wang,Hanqing Lv,Yuqi Zhou,Lihua Zhu,Yue Hu,Tetsuro Majima,Heqing Tang
Perfluorooctanoic acid (PFOA) is a persistent organic pollutant that has received concerns worldwide due to its extreme resistance to conventional degradation. A mechanochemical (MC) method was developed for complete degradation of PFOA by using alumina (Al2O3) and potassium persulfate (PS) as comilling agents. After ball milling for 2 h, the MC treatment using Al2O3 or PS caused conversion of PFOA to either 1-H-1-perfluoroheptene or dimers with a defluorination efficiency lower than 20%, but that using both Al2O3 and PS caused degradation of PFOA with a defluorination of 100% and a mineralization of 98%. This method also caused complete defluorination of other C3∼C6 homologues of PFOA. The complete defluorination of PFOA attributes to Al2O3 and PS led to the weakening of the C–F bond in PFOA and the generation of hydroxyl radical (•OH), respectively. During the MC degradation, Al2O3 strongly anchors PFOA through COO––Al coordination and in situ formed from Lewis-base interaction and PS through hydrogen bond. Meanwhile, mechanical effects induce the homolytic cleavage of PS to produce SO4•–, which reacts with OH group of Al2O3 to generate •OH. The degradation of PFOA is initiated by decarboxylation as a result of weakened C–COO– due to Al3+ coordination. The subsequent addition of •OH, elimination of HF, and reaction with water induce the stepwise removal of all carboxyl groups and F atoms as CO2 and F–, respectively. Thus, complete defluorination and mineralization are achieved.
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Environmental Science-Nano
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2019
·Vol. 6
·期 7
·2241-2252
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IF 7.704
Jinxi Feng,Jingxiang Sun,Xiaosheng Liu,Jinzhu Zhu,Ya Xiong,Shuanghong Tian
Two electrocatalysts Pt and RuO2 were directionally co-loaded on the nano-piezomaterial t-BaTiO3 by a two-step process: the alkali deposition–oxidation of RuO2 followed by the selective photo-reduction deposition of Pt. It was found that both Pt and RuO2 could considerably improve the piezo-degradation efficiency of t-BaTiO3 for pollutants. For the biorefractory pesticide tricyclazole, RuO2/t-BaTiO3/Pt possessed a piezo-degradation kinetic constant of 0.032 min−1. The rate constant was 3.11, 2.56 and 2.58 times that of t-BaTiO3, Pt/t-BaTiO3 and RuO2/t-BaTiO3, respectively. Moreover, the rate constant of RuO2/t-BaTiO3/Pt was greater than the sum (0.025 min−1) of the rate constants of two single-loaded materials, Pt/t-BaTiO3 and RuO2/t-BaTiO3. This indicates that co-loaded Pt and RuO2 in RuO2/t-BaTiO3/Pt have a synergistic enhancement effect on the piezo-degradation. By analyzing the kind and amount of the reactive oxygen species (˙OH, 1O2, ˙O2− and H2O2) from these nano-piezocatalytic systems, it was inferred that Pt acted as a cathodic- and anodic-like catalyst while RuO2 acted as an anodic-like catalyst. The mechanism of the synergistic catalysis for co-loaded Pt and RuO2 was similar to the principle of an electrolytic reactor, in which Pt and RuO2 were its two catalytic nano-electrodes and the power was from the piezo-potential of t-BaTiO3.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Hui Li,Yanlin Zhang,Qian Zhang,Yifei Wang,Yanping Fan,Xin Gao,Jing Niu
In our work, Z -scheme Ag 3 PO 4 /NG/WO 3 composites were fabricated via a facile deposition approach, which was used in the photocatalytic degradation of indomethacin (IDM) under visible light irradiation. The as-prepared Ag 3 PO 4 -based photocatalysts were characterized by X-ray diffraction analysis, scanning electron microscopy, transmission electron microscope , Fourier transform infrared, X-ray photoelectron spectroscopy and UV–visible diffuse reflectance spectroscopy in order to determine the chemical structure , morphological feature and optical performance. From the degradation experiments of IDM, the Ag 3 PO 4 /NG/WO 3 composite exhibited the highest photocatalytic activity and stability, and its kinetics constant was ~8 times of pure Ag 3 PO 4 . Furthermore, reactive species trapping experiment, electron spin resonance , liquid chromatography-mass spectrometry, total organic carbon , photoelectrochemical measurement and photoluminescence spectra were applied to analyze the possible degradation pathways and photocatalytic mechanism of IDM. The results indicated that the visible-light photocatalytic degradation of IDM using Ag 3 PO 4 /NG/WO 3 conformed to a Z -scheme photocatalysis mechanism, further facilitating the photoinduced charge carriers separation, and inhibiting the recombination of photoinduced electron-hole pairs. It also confirmed that the holes, OH and O 2 – radicals generated in Z -scheme system played the significant roles during the photocatalytic degradation of IDM.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yuwei Pan,Minghua Zhou,Jingju Cai,Yusi Tian,Ying Zhang
Sulfamethazine (SMT) is extensively used as growth promoters and antibacterial drugs. In this study, premagnetized Fe 0 was used to catalyze H 2 O 2 decomposition (pre-Fe 0 /H 2 O 2 ) in the presence of nitrilotriacetic acid (NTA) to remove SMT at neutral pH conditions. In all, 30.3% and 99.8% of SMT were removed by the pre-Fe 0 /H 2 O 2 process (60 min) and the pre-Fe 0 -NTA/H 2 O 2 process (30 min), respectively. The removal rate of SMT in the pre-Fe 0 -NTA/H 2 O 2 process was 2.5 times larger than that in the Fe 0 -NTA/H 2 O 2 process. Electron paramagnetic resonance signals indicated that more radicals were generated in the pre-Fe 0 -NTA/H 2 O 2 system. SMT and NTA and their degradation by-products adsorbed on pre-Fe 0 reduced the contact angle of the particle and prevented the formation of Fe 3 O 4 on the particle surface, thus accelerating Fe 0 corrosion. Tafel scan images confirmed the enhancement of Fe 0 corrosion in the presence of NTA and magnetic field. The Fe 0 corrosion rate (10 9 ) after 20 min of reaction was 6.61 cm/s in pre-Fe 0 -NTA/H 2 O 2 , much higher than that in Fe 0 /H 2 O 2 (0.73 cm/s), pre-Fe 0 /H 2 O 2 (1.47 cm/s) and Fe 0 -NTA/H 2 O 2 (2.94 cm/s). Pre-Fe 0 -NTA/H 2 O 2 could also keep the fast SMT removal with eight consecutive runs without the addition of pre-Fe 0 and NTA and presented high efficiency for SMT removal in real municipal wastewater .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Chao Liu,Liwei Chen,Dahu Ding,Tianming Cai
Conversion of agricultural biomass waste to value-added biochar based catalysts receives tremendous interests because it falls into the scope of resource recycle concept. In this work, a magnetic nitrogen doped biochar-supported CoFe 2 O 4 composite (MNBC) was synthesized by using rice straw, an abundant agricultural waste as the precursor. The prepared catalyst exhibited excellent performance in catalytic degradation of metolachlor (MET), a broad-spectrum chloroacetanilide herbicide, by coupling with peroxymonosulfate (PMS). The pyrolysis temperature played a significant role in the activity of the resultant catalysts. Among others, MNBC 800 catalyst performed the best stability and reusability. In-situ (EPR) analysis revealed that SO 4 •− , •OH and 1 O 2 participated into the degradation process and the SO 4 •− was the major contributor. The degradation was promoted at neutral and weak basic conditions, whilst significantly inhibited at strong basic condition (pH = 11). Eleven degradation intermediates were successfully identified through liquid chromatography – quadrupole time-of-flight – mass spectrometer (LC-Q-TOF-MS). The degradation mainly occurred via hydroxylation, dechlorination, and dealkylation reactions. Additionally, though the degradation was greatly inhibited in real wastewater , it was not remarkably influenced in river and groundwater, implying its applicability in river/groundwater remediation. Eventually, the easy separation and low toxicity make the catalyst promising for the degradation of MET from several aquatic systems. This study would pave the way to the catalytic degradations of organic pollutants by low-cost biochar based catalysts.
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CHEMOSPHERE
·
2019
·
IF 5.108
Jingchun Yan,Yudong Chen,Weiguo Gao,Yun Chen,Linbo Qian,Lu Han,Mengfang Chen
A high catalytic system using Cu layered double hydrotalcite (Cu(II)-Mg(II)-Fe(III)LDHs) and hydrogen peroxide (H 2 O 2 ) was developed for the degradation of ethylbenzene. It was identified that the degradation efficiency of ethylbenzene (0.08 mmol L −1 ) and TOC removal were 96.1% and 39.7% respectively in the presence of 0.1 g L −1 Cu(II)-Mg(II)-Fe(III)LDHs with (Cu 2+ + Mg 2+ )/Fe 3+ molar ratio of 5.0 and 0.16 mmol L −1 H 2 O 2 in 6.0 h. Based on ESR and XPS data, hydroxyl radicals (•OH) were the predominant free radical specials generated from the catalytic decomposition of H 2 O 2 for the degradation of ethylbenzene. The redox of Cu(II)/Cu(III) on the layered Cu(II)-Mg(II)-Fe(III)LDHs surface active sites accounted for the formation of •OH radicals and the cycle of Cu(II) in the Cu(II)-Mg(II)-Fe(III)LDHs/H 2 O 2 system were proposed.
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