JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yamei Huang,Jing Li,Peiyao Du,Xiaoquan Lu
Photocatalysis utilizing solar energy is a promising strategy for mitigating energy crisis and environmental pollution. Exploring a cost-effective, stable, eco-friendly, and efficient photocatalytic system is extremely urgent. Herein, copper encapsulated within nitrogen-doped carbon nanosphere (Cu@N C) possessing a unique core-shell structure with high catalytic activity was prepared by ion-exchange and pyrolysis using resin as support. The protective carbon shell can prevent the leaching of metal ions and deactivation of the catalyst. Benefiting from the special structure, Cu@N C exhibited excellent activity and durability toward the degradation of tetracycline by the activation of peroxymonosulfate (PMS). The radical trapping experiments and electron spin resonance analyses were applied to elucidate the main reactive species. This work highlights the great potential of Cu@N C core-shell nanosphere as photocatalyst , which provides a new opportunity for the remediation of environmental pollution.
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International Journal of Nanomedicine
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2021
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IF 6.4
Yarong Wang,Xueling Yan,Qiming Kou,Qi Sun,Yuexin Wang,Ping Wu,Lulan Yang,Jiaming Tang,Tao Le
Purpose Sulfamethazine (SMZ) exposed in the environment can enter the human body through the food chain and pose a serious threat to human health. Therefore, it is important to develop a rapid and sensitive method for detecting SMZ in environmental samples. In order to fastly and quantitatively detect SMZ in environmental samples, we developed a label-free fluorescent aptasensor based on specific aptamer (SMZ1S) and fluorescence resonance energy transfer (FRET) between gold nanoparticles (AuNPs) and rhodamine B (RhoB).Methods In the absence of SMZ, SMZ1S was adsorbed on the surface of AuNPs, which led to dispersion of the AuNPs in high concentration saline solution, thus effectively quenching the fluorescence of RhoB. With the increase of the SMZ concentration, the specific binding of SMZ1S and SMZ led to the aggregation of AuNPs in the presence of NaCl, which reduced the quenching of RhoB fluorescence and increased the fluorescence intensity. The sensitivity and linearity curve of the label-free fluorescent aptasensor were determined with different concentrations of sulfamethazine standard solutions. The specificity of this fluorescent aptasensor was determined by replacing sulfamethazine with different antibiotics. In addition, the actual water and soil samples were spiked and recovered.Results Under optimized conditions, the proposed fluorescent aptasensor demonstrated a good linear detection of SMZ in binding buffer from 1.25 ng mL−1 to 40 ng mL−1 and the limit of detection was 0.82 ng mL−1. The spiked recoveries for SMZ were 94.4% to 108.8% with a relative standard deviation of 1.8–10.3% in water and soil samples, respectively.Conclusion The label-free fluorescent aptasensor investigated in the current study is a promising tool to detect and quantify SMZ in water and soil samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhijia Zhu,Chenmiao Zhu,Ruiying Yang,Lingfeng Yan,Chunyan Hu,Baojiang Liu
Exploring the efficient and sustainable photocatalysts is the key pot for the improvement of photocatalytic efficiency. In this work, a series of Bi 5 O 7 I/BiOIO 3 composite materials were successfully prepared via a mild hydrothermal method to make layered BiOIO 3 nanosheets uniformly grown in-situ on the smooth surface of Bi 5 O 7 I microrods. The electronic channel at the interface constructed by the in-situ growth could drastically shorten the distance of electron transmission to accelerate the electron transfer. The formation of Bi 5 O 7 I/BiOIO 3 heterojunction was determined via the characterization of the composition and photochemical analysis. Benefited from this structure, the Bi 5 O 7 I/BiOIO 3 with the mass ratio of 1:1 exhibited over 90% efficiency in degradation of 4 different antibiotics after irradiation for 120 min. After that, 5 cycles proved that Bi 5 O 7 I/BiOIO 3 has excellent stability and reusability, which can guarantee the application in the practical process. Finally, the electron migration path and photocatalytic mechanism of the catalyst are inferred base on the capture experiment and ESR test, which proposed that h + and ·O 2 - were the primary active species in the photocatalytic process and confirmed the formation of Z-type heterojunctions between Bi 5 O 7 I and BiOIO 3 . The heterostructure with well-matched band structure enhances the separation and migration of photogenerated charges, which contributes to improve the photocatalytic activity. The design of novel photocatalyst with high efficiency and low-toxicity provides a new approach to achieve full utilization of solar energy and efficient environmental purification.
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CHEMOSPHERE
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2021
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IF 7.086
Fuyou Du,Zhan Lai,Huiyang Tang,Haiyan Wang,Chenxi Zhao
In this work, a novel BiOCl/Cu-doped Bi 2 S 3 photocatalyst was designed to efficiently remove ciprofloxacin (CIP) with high photocatalytical activity and good stability over a wide pH range. Compared with Cu-doped Bi 2 S 3 , Bi 2 S 3 , BiOCl, BiOCl/Bi 2 S 3 , and Cu-doped BiOCl, the photocatalytical degradation rate of CIP (97.1% at 20 mg/L) over BiOCl/Cu-doped Bi 2 S 3 was enhanced by about 84.77, 44.23, 2.95, 2.27, and 1.96 times within 20 min, respectively. Notably, the BiOCl/Cu-doped Bi 2 S 3 photocatalyst also displayed high photocatalytical performance in the degradation of other antibiotics including norfloxacin, ofloxacin, and tetracycline (40 mL, 20 mg/L; 88.3%, 100%, and 95.2% of degradation rate within 30 min, respectively) under visible light irradiation. Radical trapping experiments and electron spin resonance technique indicated that superoxide radicals (•O 2 − ) and photogenerated holes (h + ) played crucial roles in the photocatalytic degradation of CIP. Finally, the possible CIP degradation pathways was proposed by detecting the CIP intermediates in photocatalytical reaction process.
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ACS Omega
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2021
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IF 3.512
Libin Wan,Huoliang Gao,Ge Yan,Haidong Gao,Mantang Chen
Molecularly imprinted polymers (MIPs) with high specific recognition capability are promising in environmental remediation. However, traditional MIPs usually show poor specific binding affinity toward templates in pure aqueous medium, thus greatly limiting their practical applications in wastewater treatment. Herein, we proposed a facile and versatile method to synthesize a water-compatible hierarchically porous MIP (HP-MIP), in which a metal–organic gel (MOG) was formed by in situ assembly and acted as a removable structural modulator. Remarkably, the integration of the MOG modulator and template imprinting defects significantly improved the specific template binding affinity of HP-MIP in water. The adsorption behavior of HP-MIP fitted well with the heterogeneous Freundlich isotherm, suggesting that HP-MIP possessed greater site heterogeneity to sildenafil than HP-NIP, which confirmed the efficiency of HP-MIP for the removal of sildenafil from water. This approach provides an important pathway to prepare water-compatible porous MIP for efficient removal of highly toxic organic pollutants from wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yi-Jing Shi,Lei Yang,Sheng-Fa Liao,Li-Guo Zhang,Zi-Cong Liao,Min-Yi Lan,Feng Sun,Guang-Guo Ying
In this study, aerobic granular sludge (AGS) was operated under high levels of ammonium for removing three fluoroquinolones (FQs), i.e., ciprofloxacin (CFX), ofloxacin (OFX), and norfloxacin (NFX) at 3, 300, and 900 µg/L, respectively. Two key objectives were to investigate the differential distribution of antibiotic resistance genes (ARGs) and mobile genetic elements (MGEs) in sludge fractions and to evaluate correlations between ARGs and MGEs to nitrifying and denitrifying bacteria. AGS showed excellent stability under the exposure of FQs, with nitrite-oxidizing bacteria (NOB) more sensitive to FQs than ammonium-oxidizing bacteria (AOB). Specific oxygen utilization rates (SOUR) showed a reduction of 26.9% for NOB but only 4.0% of the reduced activity of AOB by 3 μg/L FQs. AGS performed better removal efficiencies for CFX and NFX than OFX, and the efficiencies increased with their elevated concentrations, except at 900 μg/L FQs. The elevated FQ concentrations led to a significant enrichment of intI1 and genus Thauera , while qnrD and qnrS showed no accumulation. Compared to nitrifiers, FQs relevant ARGs and the intI1 gene preferred to exist in denitrifiers , and the abundance of denitrifiers behaved a decreasing trend with the sludge size. Two quinoline-degrading bacteria were found in the AGS system, i.e., Alicycliphilus and Brevundimonas , possibly carrying qnrS and qnrD , respectively. Their relative abundance increased with the sludge size, which was 2.18% in sludge <0.5 mm and increased to 3.70% in sludge >2.0 mm, suggesting that the AGS may be a good choice in treating FQs-containing wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Qihui Pan,Qiang Gao,Guimei Gao,Mingyang Liu,Bo Han,Kaisheng Xia,Chenggang Zhou
Herein, we report for the first time the construction of perovskite oxide catalysts on monolithic supports for peroxymonosulfate (PMS) activation to eliminate organic pollutants in wastewater. Specifically, the commercially available porous alumina ceramic (PAC) was utilized as monolithic support, on which Ca − Ti co-modified LaCoO 3 perovskites (L 1− x C x C 1− y T y O 3 ) were successfully loaded through a simple, controllable, and reagent-saving “dripping − calcination” process. The resulting monolithic catalysts (L 1− x C x C 1− y T y O 3 @PAC) featured large sizes (cm-scale), highly open porous architectures, and compositionally favorable active components, by which easy catalyst recycling, rapid mass transfer of guest species, and high yet stable catalytic performance were harvested in PMS activation for degradation of the typical antibiotic pollutant metronidazole (MNZ). By optimizing the introduction amount of Ca and Ti, the resulting L 0.8 C 0.2 C 0.4 T 0.6 O 3 @PAC showed a high turnover frequency (TOF) value of 12.6 min −1 for MNZ with a low cobalt leaching amount of 0.203 mg L −1 , which were significantly superior to the unmodified catalyst LCO 3 @PAC (TOF: 7.9 min −1 ; cobalt leaching: 1.71 mg L −1 ). Roles of Ca and Ti modifiers in the LaCoO 3 -based monolithic catalyst, degradation pathway of MNZ, and SO 4 − •/ 1 O 2 dominated catalytic mechanism were investigated and elucidated. Our work provides a promising avenue for rational design of low-cost, easily operational, and robust monolithic catalysts toward PMS activation for large-scale environmental remediation.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Haitao Li,Qiang Gao,Guanshuai Wang,Bo Han,Kaisheng Xia,Chenggang Zhou
As one of the newly emerging heterogenous catalysts for peroxymonosulfate (PMS) activation, complex hollow structured nanoreactors with multilevel interiors can significantly enhance the catalytic performance and manifest great potentiality in organic pollutant degradation. Herein, a novel yolk–shell structured CoTiO 3 @Co 3 O 4 nanoreactor was synthesized via a simple self-template method using amorphous TiO 2 nanospheres as template and CoCl 2 ·6H 2 O as cobalt source, respectively. Owing to the remarkable structural advantages and unique space confined effect, the as-synthesized CoTiO 3 @Co 3 O 4 nanoreactor exhibited a high efficiency for PMS activation, enabling 100% removal of rhodamine B (RhB; 50 mg L −1 ) in a short period of time, with a rate constant (0.1993 min −1 ) much higher relative to those of CoTiO 3 (0.0246 min −1 ) and Co 3 O 4 (0.0150 min −1 ). Moreover, this catalyst showed a low cobalt leaching (0.080 mg L −1 ) while keeping almost unchanged catalytic activity in the cyclic degradation processes. Based on ESR analysis and quenching experiments, the possible catalytic mechanism was proposed. The mineralization degree was found to be 79.5% in the RhB degradation process via TOC analysis. LC/MS was employed to identify the intermediates and corresponding degradation pathway was elucidated. Besides, CoTiO 3 @Co 3 O 4 nanoreactor was revealed to be also highly efficient in activating PMS for degradation of several other recalcitrant organic pollutants. This work may be suggestive to the design and synthesis of advanced complex hollow nanoreactors for environmental remediation.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Xiangning Han,Hong Lin,Limin Cao,Xiangfeng Chen,Luefeng Wang,Hongwei Zheng,Ziang Zhang,Tushar Ramesh Pavase,Sai Wang,Xun Sun,Jianxin Sui
Purification of antibodies has become a critical factor in antibody production. A high-purity specific antibody against antigens, especially small molecules, seems to be difficult to obtain, even with the help of a protein A affinity column, which is a conventional and broadly used ligand for the separation of antibody and non-antibody proteins. Therefore, it is urgent to develop a cheap, simple, efficient, and stable method to separate the specific antibody from other antibodies. In this study, to improve the sensitivity and accuracy of immunoassay results, enrofloxacin (ENR) was grafted onto polyethylenimine (PEI) by the abundant amino groups and then the whole ligand (ENR–PEI) was conjugated to CNBr–Sepharose 4B to prepare the affinity column for the purification of the specific antibody against ENR from polyclonal antibodies. Scanning electron microscopy and Fourier transform infrared spectroscopy verification showed that Sepharose 4B was successfully modified by ENR–PEI with excellent uniformity. The capacity of the prepared column could reach to 6.15 mg of specific antibody with high purity per milliliter resin due to the high coupling ratio (49.3:1) of ENR on PEI, and the IC50 value of the antibody after purification was 47.58 ng/mL with a lowest limit of detection (IC10) of 1.099 ng/mL—18 times lower than those of the antibody purified through the protein A column. All the results showed that this new kind of resin could be used as the potential ligand in the purification of the trace-specific antibody against antigens in complex mixtures with high efficiency and specificity.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Xiaoxiao Wei,Yuzhi Wang,Jing Chen,Fangting Xu,Ziwei Liu,Xiyan He,Heqiong Li,Yigang Zhou
The ecological and human health threats brought by emerging pollutants are increasingly serious. Development of efficient removal methods is urgent. Herein, seven deep eutectic solvents (DESs) composed by quaternary ammonium salts and lactic acid or glycolic acid were synthesized and used to regulate magnetic (Fe 3 O 4 ) metal organic framework (MUiO-66-NH 2 ) composites. The obtained nanoparticles (named as DES-MUiO-66-NH 2 ) were used as adsorbents to adsorb pharmaceuticals and personal care products (PPCPs). Langmuir isotherm model and pseudo-second-order kinetics model were suitable to analyze the adsorption process of DES-MUiO-66-NH 2 to PPCPs, indicated that the adsorption of PPCPs was chemisorption on homogeneous surface of DES-MUiO-66-NH 2 adsorbents. Under the optimal conditions, the adsorption capacity of DES-MUiO-66-NH 2 toward ofloxacin and mefenamic acid reached up to 97.60 and 79.22 mg/g, respectively. Mechanism exploration indicated that DES-MUiO-66-NH 2 selectively adsorbed PPCPs through electrostatic interaction, chelation, π-π stacking, hydrophobic interaction and hydrogen bonding. Density functional theory proved the chelation through theoretical calculation. Selective experiments manifested that the structures of DESs directly determined the specificity of DES-MUiO-66-NH 2 for different PPCPs, and the investigation of structure–activity relationship provided new ideas for designing efficient tailor-made adsorbents for PPCPs. The proposed PPCPs removal approach focused on the guiding role of DESs in selective adsorption. And this green DESs regulation idea provided more options for the synthesis of high-efficiency and functional adsorbents for emerging pollutants.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Haiping Liu,Jing Liang,Shuai Fu,Li Li,Jiehu Cui,Penghui Gao,Fengying Zhao,Jianguo Zhou
Exploiting metal-free cocatalysts is of huge interest for photocatalytic technology in environmental wastewater remediation and water splitting fields. The N doped carbon quantum dots (NCDs) modified defect-rich g-C 3 N 4 (DCN) was prepared through impregnation method. The structural, optical and electronic properties of NCDs/DCN were systematically investigated. The NCDs/DCN with outstanding visible light absorption, narrowed gap and electron transfer ability were conducive to combined pollutions photocatalytic removal and simultaneous H 2 production and rhodamine B (RhB) degradation. The resulting NCDs/DCN performed much higher removal efficiency in different combined pollutions systems containing OFL/Cr (VI), BPA/Cr (VI) and CIP/Cr (VI) than in single system owing to the synergistic effect between organic pollution oxidation and Cr (VI) reduction. The free-radical quenching experiments, spectral technology and electron spin resonance (ESR) confirmed that Cr(VI) can be reduced by the conduction band (CB) electrons, and the h + and O 2 − radicals dominated OFL degradation. The optimized NCDs/DCN displayed excellent simultaneously photocatalytic H 2 production activity and RhB degradation with the H 2 evolution rate of 3.68 μmol‧h −1 ‧g −1 and 100% RhB removal efficiency. The photocatalytic activity of simultaneous combined pollutions removal and synergistic H 2 generation and RHB degradation provides a promising strategy for real wastewater remediation applications and energy utilization.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Yangcheng Ding,Wenli Jiang,Bin Liang,Jinglong Han,Haoyi Cheng,Muhammad Rizwan Haider,Hongcheng Wang,Wenzong Liu,Shuangjiang Liu,Aijie Wang
The biological treatment of antibiotic-containing wastewater is a mainstream process, but the antibacterial activity from the persistence of antibiotics would inhibit the biological activity and function of wastewater treatment plants and lead to the risk of transmission of antibiotic resistant bacteria and genes. In this study, UV photolysis was selected as an appropriate pretreatment technology for antibiotic-containing wastewater. It could decompose many kinds of antibiotics and was not inhibited by the coexisting organics in wastewater. The antibacterial activities of five kinds of antibiotics, which were eliminated with UV irradiation, exhibited a significantly positive correlation with their parent compound concentrations. The photodecomposition of the main functional groups in antibiotics contributed to the elimination of antibacterial activity. Defluorination was the main pathway to eliminate the antibacterial activity of antibiotics containing a fluorine substituent (e.g., florfenicol and ofloxacin), while the photoinduced opening of the β-lactam ring was the most efficient route to eliminate the antibacterial activity of β-lactam antibiotics (e.g. cefalexin, amoxicillin and ampicillin). These results demonstrated that UV photolysis could be adopted as an efficient and promising pretreatment strategy for the source control of antibiotic antibacterial activity by the decomposition of antibiotic functional groups before the biological treatment unit.
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危险品化学品经营许可证（带存储）