MOLECULES
·
2023
·Vol. 28
·期 8
·3542
·
IF 4.6
Qing Liu,Chao Yan,Yan Wang
Applications of submicron-scale particles are of rising interest in separation science due to their favorable surface-to-volume ratio and their fabrication of highly ordered structures. The uniformly dense packing beds in columns assembled from nanoparticles combined with an electroosmotic flow-driven system has great potential in a highly efficient separation system. Here, we packed capillary columns using a gravity method with synthesized nanoscale C18-SiO2particles having diameters of 300–900 nm. The separation of small molecules and proteins was evaluated in the packed columns on a pressurized capillary electrochromatography platform. The run-to-run reproducibility regarding retention time and peak area for the PAHs using a column packed with 300 nm C18-SiO2particles were less than 1.61% and 3.17%, respectively. Our study exhibited a systematic separation analysis of small molecules and proteins based on the columns packed with submicron particles combined with the pressurized capillary electrochromatography (pCEC) platform. This study may provide a promising analytical approach with extraordinary column efficiency, resolution, and speed for the separation of complex samples.Keywords:submicron scale particles;pressurized capillary electrochromatography;separation
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Wenjun Zhu,Xiaohua Zuo,Xiaofei Zhang,Xiangyi Deng,Deng Ding,Chunlei Wang,JunTao Yan,Xiaobo Wang,Guanghui Wang
A novel CuO–Fe 3 O 4 encapsulated in the carbon framework with abundant oxygen vacancies (CuO–Fe 3 O 4 @C) was successfully prepared by thermal conversion of Cu(OAc) 2 /Fe-metal organic framework. The as-prepared catalyst exhibited excellent peroxymonosulfate (PMS) activation performance, good recyclability and fast magnetic separation. Under optimal conditions, the added BPA (60 mg/L) could be completely removed by CuO–Fe 3 O 4 @C/PMS system within 15 min with the degradation rate constant ( k ) of 0.32 min −1 , being 10.3 and 246.2 times that in CuO/PMS (0.031min −1 ) and Fe 3 O 4 /PMS (0.0013 min −1 ) system. A deep mineralization rate of BPA (＞80%) was achieved within 60 min. The results demonstrated the synergistic effect of bimetallic clusters, oxygen vacancies and carbon framework was a key benefit for the exposure of more active sites, the electron donor capacity and the mass transfer of substrates, thereby promoting the decomposition of BPA. Capture experiments and EPR indicated that 1 O 2 was the predominant reactive oxygen species (ROSs). The degradation routes of BPA and the activation mechanism of PMS were proposed. This study offers an opportunity to develop promising MOFs-derived hybrid catalysts with tailored structures and properties for the practical application of SR-AOPs.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Hengye Li,Xingwei Han,Lin Zhang,Wenjie Yu,Wenwen Bie,Meijie Wei,Zhongxia Wang,Fenying Kong,Wei Wang
Herein, β-cyclodextrin-containing hybrid polymers (P1, P2 and P3) were prepared through crosslinking partially benzylated β-cyclodextrin (PBCD) by octavinylsilsesquioxane (OVS). P1 stood out in screening studies and the residual hydroxyl groups of PBCD was sulfonate-functionalized. The obtained P1-SO 3 Na showed greatly enhanced adsorption towards cationic MPs and maintained the excellent adsorption performance towards neutral MPs. The rate constants ( k 2 ) of cationic MPs upon P1-SO 3 Na were 9.8–34.8 times larger than those upon P1. The equilibrium uptakes of the neutral and cationic MPs upon P1-SO 3 Na were above 94.5 %. Meanwhile, P1-SO 3 Na demonstrated appreciable adsorption capacities, excellent selectivity, effective adsorption of mixed MPs at environmental levels and good reusability. These results confirmed the great potential of P1-SO 3 Na as effective adsorbent to remove MPs from water.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 19
·13716-13727
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IF 3.3
Caihong Wang,Yong Liu,Fengshen Han,Yongzhe Han,Tianyu Liu,Haitao Ren,Xu Han
Using metal-free catalysts is widely recognized as a promising approach toward wastewater remediation because of the absence of metal leaching. However, the oxidation products involved in the oxidation process and the corresponding mechanisms are still not clear. In this work, N-doped carbocatalysts (CN) were fabricated using as-prepared g-C3N4 and glucose solution, and the reactivity of the as-prepared catalysts was optimized by controlling calcination temperature. Correspondingly, increasing the calcination temperature promotes the catalytic oxidation of BPA. The positive correlations between the contents of pyridinic-N and graphitic-N and the kobs values of BPA oxidation, as well as XPS analysis indicate the important roles of pyridinic-N and graphitic-N in BPA oxidation. According to the series of characterizations of the oxidation products and Raman analysis of the reaction process, the moderately activated persulfate (PS) on the CN catalyst is the predominant species in BPA oxidation and BPA can be oxidized to BPA polymers with high selectivity by H-abstraction under alkaline conditions. This work highlights the important role of the moderate activation of PS in the polymerization of phenolic contaminants under alkaline conditions, which enriches our understanding of the oxidation of aromatic contaminants by PS under alkaline conditions.
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Environmental Progress & Sustainable Energy
·
2023
·Vol. 42
·期 5
·e14140
·
IF 2.8
Li Hua,Taozhi Cheng,Ting Wei
Advanced oxidation based on persulfate applied for the removal of organic pollutants has received widespread attention. Here, combining hydrothermal synthesis and a high-temperature calcination approach, we constructed an effective copper oxide-modified biochar from wood waste ( Ginkgo biloba rods) for the removal of bisphenol A (BPA) from contaminated waterways. The modified biochar with copper oxide in its structure (CuO/BC) exhibited a densely arranged needle-shaped structure different from pristine timber waste biochar (BC). CuO/BC can activate persulfate efficiently, and the removal rate of BPA could reach 100% within 20–30 min, approximately three times higher than that of BC. Moreover, CuO/BC was more suitable for treating BPA wastewater under alkaline conditions. The stability of CuO/BC, reaction intermediates, and possible degradation pathway were investigated. These results demonstrate the potential of the application of CuO/BC for organic wastewater treatment and shed light on a new approach to develop wastewater treatment materials that are carbon-based and cost-effective.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jianhua Qu,Zhuoran Li,Zhihuan Wu,Fuxuan Bi,Shuqi Wei,Min Dong,Qi Hu,Yifan Wang,Hui Yu,Ying Zhang
Currently, functional materials-based soil remediation focused on the stabilization of heavy metals and organics to inhibit their migration, however, the possible second release of these pollutants caused by soil condition variation attracts broad attention. Herein, β-cyclodextrin functionalized magnetic sodium alginate microspheres (MSA-CD MW ) were fast and facilely synthesized through microwave-assisted one-pot method for synchronous detachment of Pb and BPA from contaminated soil. The obtained MSA-CD MW presented wide pH adaptability and fast capture for Pb(II)/BPA with superior adsorption capacity of 369.03/165.37 mg/g. Furthermore, the effects of material dosage and soil pH on the remediation ability of MSA-CD MW were explored in detail. After adding 5% MSA-CD MW into the contaminated soil for 3-round successive remediation (12 h for each round), the amount of extractable Pb and total BPA was simultaneously decreased by 56.30 and 0.78 mg/kg, respectively. Meanwhile, the quantity of exchangeable and carbonate bound Pb was significantly decreased to 7.13% with transformation into relatively stable fractions. A series of characterizations revealed that ion exchange, pore filling, complexation, and electrostatic attraction were responsible for Pb binding, while MSA-CD MW could capture BPA through host-guest interaction by the hydrophobic cavity of β-cyclodextrin. Additionally, recovery and floatation results revealed that the MSA-CD MW could be easily separated from the soil using magnets even at extreme drying and wetting conditions, thus providing a novel, fast, and eco-friendly strategy for effective remediation of heavy metals and organics contaminated soil.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 11
·5420-5430
·
IF 3.3
Qi Guo,Jihong Xu,Rui Tang,Yulin Min,Zhenhu Hu,Penghui Shi
In the degradation process of organic pollutants, compared with the free radical pathway, the non-radical pathway shows the advantages of mild oxidation ability, strong anti-interference, and adaptation to different pH values. In this study, a manganese–nitrogen co-doped porous carbon (Mn–N@C-1) with high nitrogen content was prepared to improve the contribution rate of non-radical pathways to the degradation process of organic pollutants. The high performance of Mn–N@C-1 is attributed to the formation of Mn–Nx sites between Pyridine N and Mn, which can effectively oxidize organic pollutants in water (phenol, bisphenol A, 2,4-dichlorophenol). In addition, the catalyst exhibits high catalytic activity over a wide pH range (pH = 3–9) and has good immunity to inorganic anions. Moreover, the Mn–Nx site and graphitic-N are considered to be the generation sites of singlet oxygen, and the role of metastable Mn–N@C-1/PMS* complexes in the electron transfer process is explored. Overall, this study explores the crucial role of non-radical pathways in the degradation of organic pollutants by carbon-based materials.
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Analytical Methods
·
2023
·Vol. 15
·期 12
·1546-1552
·
IF 3.1
Yucui Hou,Xiaoling Lu,Jie Yang,Chunhua Tang,Hanbing Jiang,Tongji Cai,Meilun Chen,Zheng Wei,Peng Yu
Testosterone is a steroid hormone that plays an indispensable role in the normal metabolism of organisms. However, exogenous testosterone, even as low as nmol L−1, will harm the human body due to accumulation. In this study, we developed an unlabeled fluorescent sensor for testosterone based on SYBR Green I. SYBR Green I is a fluorescent dye that can be embedded into the G-quadruplex of the testosterone aptamer T5. The fluorescence quenching effect is utilized to achieve quantitative detection, which occurs by the competition between testosterone and SYBR Green I for the T5 aptamer binding sites. In this work, we optimized the detection conditions to make the fluorescent sensor more sensitive and verify the specificity, linear range, and detection ability in the buffer and real water samples. The sensor's LOD and LOQ values were 0.27 nmol L−1 and 0.91 nmol L−1, respectively, while the detection range was linear from 0.91 nmol L−1 to 2000 nmol L−1. According to the results, the sensor shows high specificity and good performance even in real sample detection such as tap water and river water, providing an alternative method for the quantitative detection of testosterone in the environment, which is more convenient and efficient.
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Water
·
2023
·Vol. 15
·期 4
·830
·
IF 3.4
Shuaiguo Li,Kejian Tian,Qing Qiu,Yue Yu,Han Li,Menghan Chang,Xuejian Sun,Jinming Gu,Fenglin Zhang,Yibing Wang,Hongliang Huo
As a widespread pollutant, bisphenol A (BPA) has created a serious threat to ecosystem and human health. Therefore, expanding the available microbial resources used to screen highly efficient BPA-degrading bacteria with BPA as the sole carbon source is very important for the removal of this pollutant from the environment. In this study, the BPA degradation rate ofPseudomonassp. P1 to 30 mg/L was 96.89% within 120 h. Whole genome sequencing showed that the genome of strain P1 was composed of a single circular chromosome with a full length of 6.17 Mb, which contained 5636 predicted coding genes. Comparative genomic analysis showed that strain P1 contained 210 functional genes related to BPA degradation. It was confirmed that BPA degradation genes ferredoxin (bisdA), P450 (bisdB),CotAandLacin strain P1 were highly expressed under the induction of BPA. Combined with the identification of metabolites, the route of BPA degradation byPseudomonaswas proposed. A new metabolite, 4-vinylphenol, was detected for the first time in pathway Ⅰ. In pathway Ⅱ, BPA is directly oxidized to phenol and 4-isopropenyl phenol in the presence of laccase, which is rarely reported in the process of bacterial degradation of BPA. This study confirmed that strain P1 had good tolerance to various environmental factors at the gene level and enriched the degradation mechanism of BPA.Keywords:Bisphenol A;Pseudomonas;whole genome;biodegradation
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 8
·3551-3567
·
IF 4.5
Yang Xia,Wei Songrui,Ma Xilong,Gao Zhuwei,Huang Wei,Wang Dun,Liu Zhongxin,Wang Jieqiong
The photothermal process exhibits the largest energy conversion efficiency among all solar energy utilization processes. In this study, a core–shell CoTiO 3 @MnO 2 (CTM) composite photothermal catalyst was synthesized by supporting MnO 2 on CoTiO 3 by hydrothermal synthesis. Binding to peroxymonosulfate (PMS) heterogeneous catalyst removed tetracycline in wastewater. The new catalyst was characterized by FT-IR, UV–Vis, XRD, BET, SEM, TEM, and so on. Kinetic analysis showed that CTM activated PMS at a rate of 3.2 and 3.5 times higher than that of pure light and heat conditions, with complete degradation of tetracycline (TC). Since the outer MnO 2 layer converted the absorbed solar energy into thermal energy, PMS was activated to generate active species while performing electron transfer, which resulted in a considerably improved catalytic efficiency. To prove the wide applicability of the catalyst, other pollutants were degraded, including bisphenol A (BPA), metronidazole (MNZ), and methyl orange (MO). The three pollutants were degraded within 40 min. Finally, our findings demonstrated the mechanism of the photothermal degradation process and provided a novel approach for environmental remediation using renewable solar energy.
Graphical Abstract In this paper, the degradation efficiency of CoTiO 3 was improved by loading MnO 2 on CoTiO 3 . Binding to peroxymonosulfate (PMS) heterogeneous catalyst activation for the catalytic degradation of tetracycline. It was found by experiments that the core-shell structure of the composite material CoTiO 3 @MnO 2 had better photothermal catalysis efficiency than photocatalysis and thermal catalysis.
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ACS ES&T Water
·
2023
·
IF 5.3
Yuanbo Zhou,Yang Yu,Qiang Wang,Qian Ma,Fei Huang,Chang Xing,Qiuyue Yi,Yongjun Zhang
Nitrogen doping can enhance the catalytic activity of carbon materials for activating peroxymonosulfate (PMS). The structure of nitrogen may strongly influence the generation of reactive oxygen species (ROS). However, few studies have focused on the methods for measuring ROS concentrations, making it difficult to assess the role of nitrogen species in PMS activation. Herein, we synthesized a series of nitrogen-doped waste-tire carbon and established a kinetic model with probes to estimate the ROS concentrations. Waste-tire carbon was doped with nitrogen via vibration milling and calcination, which generated the structures of graphitic N and pyridinic N. Both radical (•OH, SO4•–) and nonradical (1O2) species were discovered by electron paramagnetic resonance. The calculations with the kinetic model revealed that 1O2 was the main ROS. Besides, combined with the density functional theory, graphitic N was suggested to be responsible for the generation of 1O2. This work provides a green catalyst developed from solid waste and an effective protocol to monitor the ratios of ROS in the degradation of pollutants with PMS.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Binghong Chen,Jing Wang,Renjie Li,Hongjun Lin,Bisheng Li,Liguo Shen,Yanchao Xu,Meijia Zhang
Integration of sulfate radicals-based advanced oxidation processes (SR-AOPs) with separation membranes has enthralled considerable attentions because it can remove persistent toxic micropollutants in a low-energy and cost-effective manner. However, fabrication of such an integrated membrane simultaneously with excellent self-cleaning property, catalytic capability and long-term durability remains a challenge. Herein, for the first time, CoFe 2 O 4 (CFO) and Mn 3 O 4 (MO) nanoparticles were anchored on ultrathin graphitic carbon nitride (UCN) nanosheets via a solvothermal method to prepare heterogeneous Fenton-like catalysts (MO/CFOUCN). Systematic characterizations demonstrated the successful preparation of powder catalysts with favorable degradation ability. Notably, the optimal composite catalyst possessed satisfactory degradation (94.5 %) and kinetic rate (0.1367 min −1 ) for norfloxacin (NOR) within 30 min. Thereafter, an integrated MO/CFO/UCN@P membrane was fabricated by vacuum-assisted filtration of the catalyst on a supporting membrane surface. It was interestingly found that, benefiting from the synergistic effect of in-situ oxidation and membrane filtration, activating peroxymonosulfate (PMS) endowed the membrane with high removal rates (over 91.8 % for tetracycline, bisphenol A, humic acid (HA)) and high permeation flux (332.7 L·m −2 ·h −1 ) driven solely by gravity. Significantly, the membrane achieved a flux recovery rate of 91.9 % with the assistance of PMS after filtering HA solution. Furthermore, quenching experiments and electron paramagnetic resonance (EPR) tests confirmed that both radical and nonradical pathways contributed to the mineralization of NOR. Based on the detection of intermediates in the degradation process, potential NOR degradation pathways were proposed. Overall, this study provided new ideas about integrating Fenton-like catalysts with membrane technology for removal of persistent organic pollutants.
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