ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Jizhong Wu,Waqas Ahmad,Qin Ouyang,Jingui Zhang,Mingming Zhang,Quansheng Chen
Diethylstilbestrol (DES), an endocrine disrupting chemical, has been linked to serious health problems in humans. In this work, a regenerative flexible upconversion-fluorescence biosensor was designed for the detection of DES in foodstuffs and environmental samples. Herein, amino-functionalized upconversion nanoparticles (UCNPs) were synthesized and immobilized on the surface of a flexible polydimethylsiloxane substrate, which was further modified with complementary DNA and dabcyl-labeled DES aptamer. The fluorescence resonance energy transfer (FRET) system was established for DES detection between dabcyl and UCNPs as the acceptor and donor pairs, respectively, which resulted in the quenching of the upconversion luminescence intensity. In the presence of a target, the FRET system was destroyed and upconversion fluorescence was restored due to the stronger affinity of the aptamer toward DES. The designed biosensor was also implemented in a dual-mode signal readout based on images from a smartphone and spectra from a spectrometer. Under the optimized experimental conditions, good linear relationships were achieved based on imaging (y = 53.055x + 36.175, R2 = 0.9851) and spectral data (y = 1.1582x + 1.9561, R2 = 0.9897). The designed biosensor revealed great practicability with a spiked recovery rate of 77.91–97.95% for DES detection in real environment and foodstuff samples. Furthermore, the proposed biosensor was regenerated seven times with an accuracy threshold of 80% demonstrating its durability and reusability. Thus, this biosensor is expected to be applied to point-of-care and on-site detection based on the developed portable smartphone device and android application.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mingxia Sun,Juanjuan Feng,Jiaqing Feng,Haili Sun,Yang Feng,Xiangping Ji,Chunying Li,Sen Han,Min Sun
To improve the extraction efficiency of carbon fibers (CFs) toward organic pollutants, TiO 2 nanorod arrays (NARs) were grown in situ on CFs. Subsequently, biochar nanospheres and covalent organic framework nanospheres were separately introduced to functionalize the NARs. A sequence of materials was produced by regulating the reactant concentrations and characterized using a scanning electron microscope, an X-ray photoelectron spectrometer, an X-ray diffractometer, a Raman spectrometer, and a specific surface area analyzer. The materials were then deposited into separate poly(etheretherketone) tubes for in-tube solid-phase microextraction (IT-SPME). These tubes were evaluated with different types of organic pollutants (polycyclic aromatic hydrocarbons (PAHs), estrogens, bisphenols, and phthalate esters) using a combination of high-performance liquid chromatography and IT-SPME, and they exhibited diverse extraction performance. The extraction mechanism of each material is carefully discussed, and the structure–performance relationship is also summarized based on the chemical structures and extraction properties of the materials. The most efficient extraction materials for different analytes were discovered and used to develop analytical methods. Three online methods were used to sensitively detect PAHs, estrogens, and bisphenols in real water samples, respectively. Satisfactory results were obtained, including enrichment factors up to 6784, detection limits as low as 0.001 μg L −1 , linear ranges of 0.003–15.0 μg L −1 , and relative standard deviations ranging from 0.2% to 15.2%. The results indicate that these methods have some advantages over previous material-based methods.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xuyao Niu,Qina Yang,Zheng Wang,Yongjian Zhu,Chi Zhang,Ping Liang,Zhonghua Zhang
Copper-based catalysts for persulfate-based oxidation are desired due to the low toxicity. Herein, nanoporous copper materials were fabricated by dealloying the aluminum-copper (Al-Cu) alloys. Bicontinuous interpenetrating ligament–channel structures containing zero-valent copper (Cu 0 ) network with trace Cu 2 O on the surface were obtained by adjusting the dealloying conditions. The as-dealloyed nanoporous copper catalysts exhibited superior catalytic performances in peroxymonosulfate (PMS) activation towards the degradation of bisphenol A (BPA), compared with the commercial Cu 0 and Cu 2 O nanoparticles or counterparts prepared by liquid precipitation methods. The unique structures of nanoporous copper provide more exposure of active sites and pathways for mass transfer. In addition, the copper network with good conductivity favors the electron transfer, and the ligaments with high-density low-coordinated sites are ready to interact with PMS . Assisted by the simulated sunlight, the degradation efficiency was greatly improved through photochemical oxidation, due to the synergistic effect of light irradiation and PMS. The free hydroxyl (•OH) and sulfate (SO 4 •− ) radicals mainly contributed to the degradation of BPA in the chemical oxidation, while •OH, SO 4 •− and singlet oxygen ( 1 O 2 ) dominated the decomposition in the photochemical reaction. This study suggests that dealloying is an effective method for fabricating catalysts for persulfate-based oxidation, providing new insight in developing highly active catalysts for wastewater purification.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Cong Pan,Libin Fu,Fenna Lide,Yaobin Ding,Chengjun Wang,Jia Huang,Shaobin Wang
Reduction of bromate (BrO 3 − ) by various technologies has been extensively investigated, while the fate of oxygen and bromine atoms in BrO 3 − in these processes has been largely ignored. In this study, reduction of BrO 3 − by Fe(II) ions was investigated under various conditions via electron spin resonance (ESR), laser flash photolysis (LFP), probe of phenol and quenching experiments. It was found that reduction of BrO 3 − by Fe(II) ions produced HO•, O 2 • − and reactive bromine species (eg., Br• and Br 2 • − ). HO• and O 2 • − were generated from release of one/two oxygen atoms in BrO 3 − and its reduction intermediates (BrO 2 − and BrO − ) at one time, while Br• and Br 2 • − were generated from activation of hypobromous acid by Fe(II) and reactions of HO• with formed Br − . Due to the formation of these reactive species, the tested ten organic pollutants with diverse structures can be efficiently degraded, which including carbamazepine (CBZ), ibuprofen, phenol, benzoic acid, paracetamol, bisphenol a, 4-chlorophenol, oxcarbazepine, diclofenac and sulfamethoxazole. CBZ degradation intermediates by BrO 3 − /Fe(II) system were specially identified by liquid chromatography (LC)-mass spectrometry (MS), and three pathways of hydroxylation/nitrosylation, ring contraction-amine cleavage and bromination for CBZ degradation were proposed accordingly. This study might shed new fundamental insights to bromate reduction and its implication for transformation of co-existed organic pollutants.
✓ 已验证
产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2021
·
IF 7.514
Qingyi Wei,Peiyao Zhang,Hongbin Pu,Da-Wen Sun
Trace amounts of 17 β -estradiol (E2) in food and the environment poses a threat to human health, which has created the demand for sensitive analytical methods to detect E2. In this study, a novel fluorescent aptasensor was developed for sensitive detection of E2 based on double-chain hybridization between carbon quantum dots-labelled with E2 aptamer (CQDs-aptamer) and Fe 3 O 4 nanoparticles modified by complementary DNA (Fe 3 O 4 -cDNA). Under the optimal conditions, the aptasensor displayed a good linear range of 10 -11 –10 -6 M for E2 with the coefficient of determination (R 2 ) of 0.996, and a low detection limit of 3.48 × 10 -12 M was obtained. Besides, the aptasensor showed high selectivity and good reproducibility for E2 detection, which was successfully applied to the sensitive detection of E2 in milk as compared with tap water and lake water with satisfactory recoveries from 85.21% to 114.80%, suggesting the great significance of this aptasensor for detecting food contaminants in the food industry.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Xintong Li,Hongxia Zhao,Baocheng Qu,Yu Tian
Environmentally persistent free radicals (EPFRs) generated under irradiation have been widely detected in soil particles, atmospheric particles and microplastic particles, but the formation of EPFRs in water is not well understood. This study investigated the formation of EPFRs on particulate organic matter (POM) in water contaminated by anthracene (Ant) under irradiation. The photoformation and decay progress of EPFRs was represented with the help of electron paramagnetic resonance (EPR) technique on both actual POM and Fe(III)-montmorillonite simulated samples. EPR signals at the range of 10 16 to 10 17 spin/g were detected and the half-life time of EPFRs stored in water was at around 16.62 h and 60.80 h, much shorter than those in the air. The g factors were all larger than 2.0040, which indicated the generation of oxygen centered EPFRs. The primary intermediates were identified by gas chromatography-mass spectrometer (GC-MS) and a possible EPFR formation pathway during Ant degradation was proposed. The interaction between Ant and POM, and the hydroxylation and carbonylation of the intermediates made contributions to the generation of EPFRs. Meanwhile, the indirect photodegradation of bisphenol A (BPA) has been demonstrated by analyzing the reactive oxygen species (ROS) and photogenerated electrons in the solution with POM containing EPFRs. It is found that hydroxyl radicals (•OH) and singlet oxygen ( 1 O 2 ) were induced and might promote the photodegration. Overall, our present study provided useful information to understand the photoformation of EPFRs on POM and their fate in aqueous environments.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Yu Han,Wei Shi,Yu Tang,Weishang Zhou,Hongxiang Sun,Jiongming Zhang,Maocang Yan,Lihua Hu,Guangxu Liu
Gonadal development is a prerequisite for the reproductive success of an organism, and might be affected by environmental factors such as emergent pollutants. Although marine crustaceans are threatened by ubiquitous emergent pollutants such as microplastics (MPs) and bisphenol A (BPA) under realistic scenarios, studies about the impacts of these pollutants on the gonadal development of crustacean species are rare. In this study, the effects of MPs and BPA, alone or in combination, on gonadal development were investigated in whiteleg shrimp ( Litopenaeus vannamei ). The results obtained demonstrated that whiteleg shrimp exposed to MPs and BPA had significantly smaller gonad-somatic index (GSI) and an obvious delay in the gonad developmental stage. In addition, exposure of whiteleg shrimp to pollutants tested resulted in a reduction in the oxygen consumption rate, elevation in the ammonia excretion rate, decline in the O: N ratio, and downregulation in the expression of metabolism-related genes, indicating significant disruptions of shrimp metabolism by the pollutants. Furthermore, in addition to a few exceptions, both the in vivo contents of gonadal development-related hormones (GIH and MIH) and the expression of genes encoding regulatory hormones ( GIH , MIH , and CHH ) were upregulated by the exposure of whiteleg shrimp to the pollutants investigated, suggesting a significant obstruction of endocrine regulation. Moreover, MP-BPA coexposure was shown to be more toxic to whiteleg shrimp than the corresponding single exposures and significantly greater amount of BPA accumulated in the gonads (both testis and ovaries) of shrimp with the coexistence of MPs, which may be caused by the Trojan horse effect and summation of the toxic impacts on common targets. In general, the data obtained in this study demonstrated that MPs and BPA at environmentally realistic concentrations significantly inhibited the gonadal development of whiteleg shrimp probably by interfering with metabolism and disrupting endocrine regulation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Gen Wang,Lei Ge,Zhuoyue Liu,Xiurong Zhu,Shengjiong Yang,Kun Wu,Pengkang Jin,Xiangkang Zeng,Xiwang Zhang
Heterogeneous activation of peroxydisulfate (PDS) by transition metal oxides offers a promising strategy for organic pollutants removal but suffers from low electron transfer efficiency. Herein, layered MgO supported CuO nanoparticles was prepared by thermal conversion of metal-phenolic networks of Cu 2+ /Mg 2+ and tannic acid. CuO nanoparticles (∼2 nm) were spatial monodispersed on layered MgO, inducing the formation of electron deficient Cu 3+ and surface oxygen vacancies and thus facilitated adsorption and activation of PDS. The electron-rich CuO/MgO hybrid catalysts manifested good catalytic performance of PDS activation for organic pollutants removal. At 0.18 g/L of CuO/MgO hybrid catalyst and 0.2 mM of PDS, complete removal of bisphenol A (BPA) was achieved with a high kinetic constant (0.1 min −1 , 50 min). Quenching experiments, electron paramagnetic resonance tests, PDS decomposition behaviors, electrochemical analysis and in situ ATR-FTIR and Raman spectroscopy revealed a nonradical pathway of electron transfer for PDS activation. The CuO/MgO hybrid catalysts exhibited wide working pH range from 3 to 11, selective oxidation capability, good resistance to halide ion and high utilization efficiency of PDS, and thus would be a promising candidate for wastewater remediation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhendong Yu,Jiachen Ma,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Rongni Dou,Xiaoxia Ye,Yongqian Shi,Minghua Liu
In this study, the S modified iron-based catalyst (S-Fe@C) for activating peroxydisulfate (PDS) was fabricated by heating the S-MIL-101 (Fe) precursor at 800 °C. The resulted S-Fe@C composite mainly consisted of carbon, Fe 0 , FeS, FeS 2 , and Fe 3 O 4 , and showed strong magnetism. Compared with Fe@C obtained from MIL-101 (Fe), the S-Fe@C exhibited much higher performance (1.5 times larger) on PDS activation and the S-Fe@C/PDS could rapidly degrade various organic pollutants in 5 min under the attack of the species of SO 4 - · , 1 O 2 , electro-transfer and Fe(IV). The S element in enhancing the PDS activation mainly involved two mechanisms. Firstly, the doped S could speed up the electron transfer efficiency, resulting in a promotion on PDS decomposition; secondly, the S 2- S 2 2- or S 0 could achieve the circulation of Fe 2+ and Fe 3+ , leading to the formation of non-radicals Fe(IV) and 1 O 2 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yanqing Cong,Wanxing Wang,Xiang Chen,Shi-Wen Lv
Nowadays efficient treatment of emerging organic contaminants is still a complex task with a big challenge. Herein, a novel dandelion-like NiCo 2 O 4 microsphere was synthesized by a simple step-by-step self-assembly strategy, and obtained NiCo 2 O 4 was then as an efficient heterogeneous catalyst to activate PS for rapid degradation of emerging organic pollutants . Importantly, as-prepared NiCo 2 O 4 -300 microsphere not only exhibited great catalytic activity , but also possessed excellent performance stability and structural stability. More significantly, developed NiCo 2 O 4 -300/PS oxidation system displayed strong degradation ability toward typical contaminants, including TC , IBP, SMX, BPA , DFC as well as OFX. TOC analyses revealed that these organic pollutants could eventually be degraded into H 2 O, CO 2 and other byproducts, and wherein degradation byproducts were low toxicity or no toxicity. During the process of PS activation over NiCo 2 O 4 -300, the redox couples of Co 3+ /Co 2+ and Ni 3+ /Ni 2+ provided major catalytic sites, and the redox couples of Ni 3+ /Ni 2+ played a bigger role. Furthermore, it was also found that both SO 4 −• and •OH were main active species in the reaction system. Even in actual water samples, proposed NiCo 2 O 4 -300/PS oxidation system still showed great performance for removing pollutants. In short, current work would provide valuable references for further research.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Xia Zhang,Xitong Yang,Bing Liu,Guifen Zhu,Jing Fan
An approach of simultaneous iodine doping and heterojunction fabricating with basic bismuth salt was proposed, Based on this, a novel I/BiOIO 3 /[Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O (I/BiOIO 3 /BHN) photocatalyst was prepared. The photocatalytic activity was evaluated by the degradation of multiple refractory pollutants (rhodamine B, methyl orange, phenol , bisphenol A, bisphenol B, bisphenol Z) in water under solar light irradiation. Compared with single photocatalyst, the optimized sample displayed the reaction rate constant of 0.1606 min −1 , which was 69.8, 11.4 and 2.2 times of individual [Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O, BiOI and BiOIO 3 , respectively. The performance improvement was attributed to the inhibition of charge carrier recombination by type II heterojunction formation and the expanded solar capture range caused by the springboard effect of iodine impurity level. The photocatalytic mechanism of I/BiOIO 3 /BHN was hole oxidation , followed by·OH oxidation. Besides, the I/BiOIO 3 /BHN photocatalyst in bulk structure with micrometer size and high-density could be easily separated and recovered by simple sedimentation, confirming its good application prospect in the wastewater treatment .
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）