JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2022
·
IF 4.383
Bing Xiao,Minghao Xu,Bin Lu,Yun Wang,Hui Liu,Rufen Chen
Economical elimination of organic pollutants from waste water has be paid more attention owing to its environmental and ecological significance. In this study, an easily achievable process to in-situ fabricate copper and co-modified Z-scheme BiOCl/Bi 2 O 3 heterojunction was proposed. The study on the formation mechanism indicated that the introduction of copper ions is favorable for the formation of Bi-based catalyst with flaky morphology while the addition C-dots makes the nanosheets loosely be packed and intercrossed each other. The composite exhibited a high degradation efficiency for Bisphenol A (BPA) and 91% of BPA was removal within 35 min under xenon lamp irradiation. The excellent photocatalytic performance was attributed to the synergistic effect of the in-situ formation Z-scheme BiOCl/β-Bi 2 O 3 heterojunction, multiple charge transfer channels including Cu 2+ /Cu + and C-dots, and efficient charge separation. The electron paramagnetic resonance (EPR) analysis and quenching tests revealed that O 2 •− play a main role in degradation of BPA. Based on the experimental results, the photo-catalytic mechanism is proposed and the degradation path of BPA is revealed.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 9
·5438-5455
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IF 4.682
Liu Boyu,Liu Moxi,Xie Zhiyuan,Li Yiru,Zhang Aibo
Metal–organic frameworks (MOFs), a new type of porous functional material, have attracted widespread attention in the field of adsorption separation, medicine, and catalysis, etc., due to their unique adjustable pore structure and large specific surface. The defective zirconium-based MOF is rich in terminal Zr–OH induced by the lack of linkers and the μ3-OH originating from the Zr cluster, exhibiting high affinity for the carboxyl and sulfonic acid groups in the dyes. We report the performance of two defective zirconium-based MOFs (MOF-808 and MIL-140C) to remove Eosin y (EY), Methyl orange (MO), and Orange g from the water. Owing to the strong affinity, larger specific surface area, and better-matched pore structure, MOF-808 exhibits higher adsorption capacity for EY and MO, with maximum adsorption capacities of 661.7 mg g −1 and 532.4 mg g −1 , respectively. The adsorption kinetics, thermodynamics, adsorption cycle performance, and adsorption mechanism of two MOFs for three dyes were investigated. Adsorption thermodynamics and XPS analysis certified that both chemical adsorption and physical adsorption occur during the adsorption process, especially chemical adsorption. Desorption and regeneration tests demonstrate that both MOF-808 and MIL-140C maintained their high adsorption capacity after four cycles, indicating two MOFs are favorable candidates for removing pollutants. Graphical abstract
In this article, the adsorption performance of MOF-808 and MIL-140C on three different sizes and structures of anionic dyes is mainly studied. The results show that MOF-808 has better adsorption performance for EY and MO. At the same time, the adsorption results show that the chemical adsorption between the adsorbate and the MOFs material plays a leading role in the adsorption, resulting in a high adsorption capacity for EY, although the EY molecule has a larger molecular size.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yizhou Chen,Yuting Bai,Lijun Meng,Wenting Zhang,Jingjing Xia,Zhiming Xu,Rui Sun,Yan Lv,Tianxi Liu
Organic solvent nanofiltration (OSN), as an emerging membrane separation technology, holds great potential in pharmaceutical and chemical applications. However, the development of such a promising technology is severely retarded by the trade-off between permeability and selectivity. Herein, we report a novel thin-film nanocomposite (TFN) membrane by incorporating hollow metal-organic frameworks (MOFs) into the metal-phenolic network (MPN) selective layer for highly efficient OSN. This nanocomposite selective layer is fabricated via an aqueous deposition of tannic acid (TA) and Fe II ions with MOFs, during which the MOFs are in-situ etched to a hollow structure. Attributed to the extra transfer channels provided by hollow MOFs, the methanol permeance of the TFN membranes increases to 24.7 L·m -2 ·h -1 ·bar -1 , exhibiting an improvement of 270% compared with the membranes without MOFs (9.1 L·m -2 ·h -1 ·bar -1 ). Meanwhile, the coordination interaction between TA and metal centers in MOFs endows excellent interfacial compatibility between MPN matrix and MOF fillers, guaranteeing a defect-free selective layer and thus high rejection for small organic molecules (>99% for Alcian blue). Furthermore, various MOFs, including ZIF-67, prussian blue (PB), and MIL-53(Al), are also employed to fabricate MPN/MOF nanocomposite membranes, proving the availability and universality of this facial aqueous deposition strategy. Additionally, we also take deep insight into the mechanism of in-situ etching based on the density functional theory (DFT) calculation to pave the way for the fabrication of TFN membranes with other hollow nanofillers. This work provides a sufficient strategy for the design and construction of novel highly efficient OSN nanocomposite membranes with excellent permeability and retention performance.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Nguyen Quang Tung,Do Thi Cam Van,Dam Xuan Thang,Nguyen Thi Kim An,Tran Thi Trang,Bui Dinh Nhi,Nguyen Phuong Thao,Le The Son,Nguyen Nhat Huy,Nguyen Trung Dung
In this study, the CuCoFe-LDH catalyst was synthesized by hydrothermal method and applied to degrade levofloxacin (LFX) by peroxymonosulfate (PMS) activation. The physicochemical properties of the synthesized samples were analyzed by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The influence of various factors such as catalyst system, pH, catalyst content, PMS , pH, and coexisting ions on the degradation of LFX was systematically investigated. The results showed that after 10 min, 94.57 % of LFX was decomposed under the conditions of 200 mg/L of catalyst, 500 mg/L of PMS, 10 mg/L of LFX, and pH 7.0. Besides, the CuCoFe-LDH/PMS system can effectively remove LFX over a wide pH range from 3.5 to 9.0. Both radical superoxide (O 2 •- ) and non-radical singlet oxygen ( 1 O 2 ) were major reactive oxygen species in the CuCoFe-LDH/PMS system. Mass spectrometry identified 16 major degradation products of LFX, and 38.43 % of LFX was mineralized after 30 min of reaction. Besides, the CuCoFe-LDH/PMS system had the ability to effectively degrade different groups of antibiotics (e.g., fluoroquinolone, tetracycline , and sulfonamide). The mechanism of PMS activation by CuCoFe-LDH and the LFX degradation pathway were proposed. Finally, testing the reusability of CuCoFe-LDH in LFX degradation showed that a decrease of nearly 7 % occurred after five consecutive cycles, suggesting its stability for practical applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yuyang Zhou,Xiaochun Wu,Jin Zhang,Zhenxing Wang
Tannic acid (TA) − 3-aminopropyltriethoxysilane (APTES) coating (TA-APTES coating) composed of abundant nanospheres with secondary reaction sites has many distinct advantages for surface modification. Herein, an in-situ growth method is proposed to generate TA-APTES nanospheres on both the outer and inner surface of polypropylene (PP) membrane. Compared with previous reported TA-APTES nano spheres coating just on the outer surface of the membrane (named PP-Su-NPs), TA-APTES nano spheres on both outer and inner surfaces prepared with this method (named PP-En-NPs) exhibits much better functional performance after secondary reactions. As a proof of concept, the TA-APTES nanospheres is functionalized by tannic acid, polyethyleneimine (PEI) and Fe 3+ to carry positive charges for absorbing anionic dyes, and the dye adsorption performance of the PP-En-NPs after the secondary reactions is 7–8 times higher than that of PP-Su-NPs. Interestingly, the functionalized coating can not only absorb anionic dyes, but also cationic dyes, and selective desorption is also realized for this functionalized coating. The possible mechanism is revealed in this study. This study will accelerate the development of the TA-APTES coating, and make it become a powerful tool for membrane modification.
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JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Chao Han,Huan Liu,Yan Wang
The preparation of polymeric-based thin film composite (TFC) membrane with high permeance and superior solvent resistance in organic solvent nanofiltration (OSN) applications always involves the consumption of toxic chemicals or high energy, which does not meet the requirements of green chemistry. In this work, intrinsic insoluble polyimide (PI) nanofiber substrates were obtained by a two-step method including electrospinning of poly (amic acid) synthesized by polycondensation reaction between various monomers and subsequent thermal imidization, and the optimized one with low thermal imidization temperature was employed as substrate for TFC membrane in strong polar aprotic solvents recovery, therefore achieving the green process. The effects of different dianhydride and diamine monomers and different thermal imidization temperatures on the solvent resistance and microscopic morphology of nanofiber substrates are also studied. The optimized monomers in this work contribute to a low-temperature imidization of PI nanofiber substrate. The solvent permeance of corresponding TFC OSN membrane with the insoluble PI nanofiber substrate reaches up to 11.2 L m −2 h −1 bar −1 with 99.7% rejection in rose bengal/DMF system, and good long-term stability. This work provides potential guidelines for developing next-generation OSN membranes under a green process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Junjie Zhang,Yongjia Hong,Xu Tang,Yong Chen,Wenran Gao,Yuncheng Cai,Ningning Dong,Jiazi Xu,Li Zhang,Quli Fan,Bin Sun
The rational design of active sites in nanocarbons are the long-term pursuit for their practical applications. However, N, as the most potential active site, still encounters the problems of low atom utilization efficiency and stability in practical environmental remediation. Herein, we successfully constructed synergistic active sites consisting of graphitic N, pyridinic N, and thiophene S in heavy S, N co-doped hollow graphene spheres (HSNGS). The HSNGS exhibited exceptional efficiency in degrading tetracycline in real water, with a turnover frequency of 6.24 min −1 , which is among the highest reported. Moreover, tetracycline dissolved in practical water could be continuously and rapidly eliminated by passing through a column filled with HSNGS, maintaining its high performance even after 40 consecutive cycles. In the synergistic active sites, graphitic N and pyridinic N species accepted electrons from peroxymonosulfate, generating singlet oxygen for tetracycline degradation. Simultaneously, thiophene S coordinated with metal ions present in the practical water, synergistically enhancing the degradation of tetracycline. Additionally, the coordinated metal ions provided protection for the synergistic active sites during peroxymonosulfate activation, preventing their oxidation and enabling the continuous and rapid degradation of tetracycline. This work opens up possibilities for the industrial application of nanocarbon materials in environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Ping Sun,Hui Liu,Mingbao Feng,Xuesheng Zhang,Yingsen Fang,Zhicai Zhai,Virender K. Sharma
This work demonstrates for the first time the potential application of a novel nonradical oxidation system consisting of N/S co-doped ordered mesoporous carbon (NS-CMK-3) and peroxymonosulfate (PMS). The results showed that the NS-CMK-3 catalyst effectively activated PMS to completely degrade pharmaceutical acetaminophen (ACT). The catalytic performance of NS-CMK-3 was ~20 and 10 times better than that of pristine CMK-3 and single N-doped one (N-CMK-3), respectively. The oxidative system could also remove other pollutants (i.e., sulfathiazole, trans -ferulic acid, orange G, and phenol). A higher content of N (5.3 at.%) and a distribution of graphite-N (28.1%) were determined in NS-CMK-3 than in N-CMK-3. The synergistic effect of N/S co-doping (i.e., graphite-N and thiophene-S) resulted in the enhanced catalytic performance. The activation of PMS by NS-CMK-3 primarily followed two nonradical pathways (i.e., singlet oxygen and catalyst surface-bound reactive PMS complexes), supported by quenching experiments and electron paramagnetic resonance measurements. The p -benzoquinone ( p -BQ) and ACTdimer were main degradation products. The removal of total organic carbon (TOC) was ≈27%, suggesting nonradicals could mineralize ACT. The NS-CMK-3 not only demonstrated superior stability owing to a removal efficiency that was still as high as 98% in the fifth recycle run, but also significantly decreased the potential effects of water constituents (e.g., Cl − , NO 3 − , HCO 3 − , and humic acid) on the removal process. The NS-CMK-3/PMS oxidative system offers a novel strategy to carry out environmental remediation via nonradical processes.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 10
·1-10
·
IF 6.232
Zhen Deshuai,Shi Sisi,Gao Chan,Kang Qing,Xiao Xilin,Grimes Craig A.,Cai Qingyun
Bi, Fe, and Ti ternary co-doped ZrO 2 (BFT-ZrO 2 ) nanocomposites have been prepared by a sol-gel process and used as both adsorbent and matrix for the enrichment and determination of small molecules by surface-enhanced laser desorption/ionization time-of-flight mass spectrometry (SELDI-TOF MS). The BFT-ZrO 2 nanocomposites not only can selectively enrich a wide variety of low-mass toxic pollutants but can also be used as an excellent matrix to enhance the laser desorption/ionization efficiency with low background noise and uniform co-crystalline film. Low limits of detection (LODs) (0.1 pg mL −1 for bisphenol A (BPA), 2 pg mL −1 for tetrabromobisphenol A (TBBPA), 0.1 pg mL −1 for alizarin (AZ), 0.001 pg mL −1 for bisphenol S (BPS), 0.01 pg mL −1 for indigo blue (ID), 0.01 pg mL −1 for pentachlorophenol (PCP), 100 pg mL −1 for estradiol (E2), 0.001 pg mL −1 for cetyltrimethylammonium bromide (CTAB), 0.1 pg mL −1 for crystal violet (CV), 1 pg mL −1 for malachite green (MG), 0.01 pg mL −1 for rhodamine B (RhB), and 0.01 pg mL −1 for perfluorooctane sulfonate (PFOS) were achieved. The relative standard deviations (RSDs) of shot-to-shot are 9.4–24% and of sample-to-sample 5.2–17%. The BFT-ZrO 2 matrix was successfully applied to the determination of TBBPA and BPA in tea samples. This method shows a new strategy for determination of toxic compounds in tea.
Graphical abstract
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2020
·
IF 4.3
Xianda Liu,Zhengxiang Zhou,Jiarui Yin,Chao He,Weifeng Zhao,Changsheng Zhao
Based on the strategy of copolymerization, methacrylatoethyl trimethyl ammonium chloride (DMC) and acrylamide (AM) copolymer hydrogel particles (PCM HPs) were prepared by precipitated droplets in-situ cross-linking polymerization, to overcome the easily fragile property of pure PDMC HPs and the low adsorption capacity of pure PAM HPs. Corn oil and deionized water were used for the reaction, which would not cause any pollutions; and the preparation process only took 40 s. Through the studies on various feeding ratios of DMC to AM, the hydrogel particles (PCM 5-1 HPs) with the mass ratio of 5:1, showed the best mechanical strength and adsorption capacity. The compression strength of the PCM 5-1 HPs was 207.7 K Pa, and no obvious mechanical loss occurred during five compression-rebound cycles. In addition, the removal ratios of anionic dyes such as amaranth red, orange G, and methyl orange were all higher than 94% (the initial dye concentration was 100 μmol/L and the adsorbent mass was 4 mg); and the adsorption capacity of orange G could reach as high as 992.63 mg/g. Meanwhile, the PCM 5-1 HPs exhibited excellent selective adsorption of anionic dyes in mixed dye solutions. Therefore, the hydrogel particles prepared by the fast and environmental-friendly method had both mechanical strength and ultrahigh adsorption capacity, which verified their practicality in the removal of anionic dyes in sewage.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Bing Xiao,Meng Wu,Yun Wang,Rufen Chen,Hui Liu
Copper(II) oxide with (0 0 1) facet-exposed nanosheets was prepared via a hydrothermal method. Due to exposure of the (0 0 1) facet, the CuO nanosheets exhibited remarkable catalytic activity towards sulfite activation and tetracycline (TC) degradation across a wide pH range (pH 3.00–9.00), with the degradation rate of TC at pH 4.51–9.00 reaching 87% in the first 5 min. This rapid degradation reaction followed the BMG kinetic model. The Cu II OH groups on the (0 0 1) facet of CuO adsorbed negative SO 3 2− to form a Cu II SO 3 − complex and generate SO 3 − radicals. Sulfite radicals were oxidized by dissolved oxygen to form SO 5 − , and then, SO 5 − transformed to SO 4 − and then HO . Both SO 4 − and HO were the main species involved in TC degradation. The utilization efficiency of sulfite reached almost 100%. After normalization of the degradation rate to the specific surface area, the degradation rate of TC in the current system was 4.84 times that obtained using a CuO nanosphere system. The potential degradation pathways of TC and the catalytic mechanism of the CuO catalyst are proposed.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Dapeng Liu,Yongliang Chen,Toan Trong Tran,Ganwei Zhang
Non-polyamide (non-PA) thin-film composite nanofiltration (TFC-NF) membranes have received tremendous attention in recent years, but their development is strongly hindered by the complicated fabrication process and the trade-off between permeability and selectivity. Here, we report a highly perm-selective non-PA TFC-NF membrane through 2-minute rapid assembly of tannic acid (TA) on hydrolyzed polyacrylonitrile (PAN) substrate via Fe 3+ intermediated regulation and coordination. The optimized membrane with a molecular weight cut off of ~390 Da showed high rejections for salts in a sequence of Na 2 SO 4 (90.2%) > MgSO 4 (83.4%) > NaCl (50.0%) > MgCl 2 (35.2%) and desirable rejections for organic pollutants (e.g. >99.0% dyes, 92.2% streptomycin and 81.8% chloramphenicol) while maintaining a pure water permeability of as high as 13.6 L·m −2 ·h −1 ·bar −1 , which clearly outperforms the reported non-PA membranes. In addition, the assembled TFC membrane showed excellent antifouling performance and reasonable structural stability against operation pressure and solution alkalinity. These results are highly promising and indicate a great potential for the membrane to be used in practical nanofiltration application, e.g. water purification and wastewater reclamation. Our work outlines the production of novel high-performance non-PA membrane with a fast fabrication process in a green chemistry context.
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