JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Jiajia Wang,Lizhi Wang,Du Zhang,You Wang,Jiawei Li,Fa Zhou,Jianhan Huang,You-Nian Liu
Herein, the covalently connected core–shell metal–organic frameworks (MOFs)@covalent-organic frameworks (COFs) hybrid materials were successfully constructed by coating the stable COF-OH shell on the NH 2 -MIL-125 core. The introduction of the NH 2 -MIL-125 core endowed the hybrid materials with high Brunauer–Emmett–Teller (BET) surface area ( S BET ) and abundant unsaturated metal sites. And the coating of COF-OH shell endowed the hybrid materials outstanding physicochemical stability and visible-light response, and suitable band gaps. Moreover, the thickness of the COF-OH shell was carefully adjusted according to the feeding amount of NH 2 -MIL-125. Impressively, the electron transfer pathway in the formed heterostructure was clarified and it was proven that a type-II heterojunction was generated between the MOFs and the COFs. The formed stable C N covalent bonds in the interfacial layer was beneficial to the photogenerated electron transfer and the electron-hole pairs separation, which greatly enhanced the CO 2 photocatalytic reduction. The product NH 2 -MIL-125@COF-3 exhibited the highest CO yield of 22.93 μmol·g −1 ·h −1 , about 2 times higher than NH 2 -MIL-125 (11.82 μmol·g −1 ·h −1 ) and 3 times greater than COF-OH (7.26 μmol·g −1 ·h −1 ). This work can provide helpful ideas for the careful design of the novel MOFs@COFs hybrid materials as well as useful exploration for the CO 2 photocatalytic reduction.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jiarong Wang,Shixiong Chen,Qinghao Zeng,Hong Jiang,Haiqing Chang,Tian C. Zhang,Xiaobao Tian,Yingqi Li,Ying Liang,Kai Wang
A miniaturized point-of-use (POU) water treatment device to achieve convenient and efficient water disinfection for remote and post-disaster areas remains a challenge. Herein, such as POU device consisted of a self-polymerized polydopamine (PDA) layer and UiO-66-NH 2 nanoparticles covered electrospun polyacrylonitrile (PAN) membrane (PAN@PDA@UiO-66-NH 2 ) with bacteria filtration and photothermal antibacterial property is successfully fabricated. The membrane achieves a good interception effect of microorganisms in water because of the synergistic pore interception and adsorption effect. A nearly 100% bacterial retention efficiency was obtained by the PAN@PDA@UiO-66-NH 2 membrane. In addition, the obtained PAN@PDA@UiO-66-NH 2 membrane exhibits nearly 100% photothermal sterilization efficiency against Escherichia coli ( E. coli ) under 6 min of 808 nm infrared irradiation (1.21 W). The great photothermal effect comes from the synergistic effect of good photothermal conversion efficiency and absorption of incident light caused by the PDA layer and rough UiO-66-NH 2 particles, respectively. Through the good filtration performance and photothermal effect of the membrane, the filtration for water containing bacteria and sterilization of membrane can be realized. Meanwhile, the membrane fouling caused by bacterial growth can be inhibited. In this way, this innovative membrane has the ability to maintain great filtration and sterilization ability during long-term operation, and thus, having great potential to be used as an effective, convenient, practical, and safe POU water-treatment device.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiaoming Xu,Guoyan Hua,Yuxuan Chen,Yanhong Zhang,Zepeng Zhang,Weiben Yang,Fuqiang Liu,Aimin Li
Traditional polyamide nanofiltration membranes suffer from permeability-selectivity trade-off limitation and unsatisfactory rejection for divalent cations. Herein, a novel dually charged membrane was constructed by incorporating positively charged UiO-66-(NH 2 ) 2 into the negatively charged polyamide layer. Thanks to the customizable nanochannels of metal-organic frameworks, the amino-rich nanochannels of UiO-66-(NH 2 ) 2 could be fabricated through a ligand replacement strategy. UiO-66-(NH 2 ) 2 played a crucial role in the enhanced rejection of divalent cations, meanwhile negatively charged polyamide surface guaranteed the efficient Na 2 SO 4 rejection. Satisfactory rejections of CaCl 2 (96.07 %) and Na 2 SO 4 (90.62 %) were achieved simultaneously by optimal TFN-D5. Meanwhile, TFN-D5 owned the greatly-improved water permeance of 19.44 LMH/bar, which was about 1.5 times better than that of the TFC-control. Calculations based on density functional theory further confirmed UiO-66-(NH 2 ) 2 rejected Ca 2+ efficiently since the migration energy barrier across UiO-66-(NH 2 ) 2 was an order of magnitude higher than that of UiO-66-NH 2 and UiO-66. Moreover, the desirable rejections were beyond 94 % towards many divalent cation salts including MgCl 2 , NiCl 2 , PbCl 2 , MnCl 2 , CdCl 2 and ZnCl 2 . Thus, this work provided an efficient way to realize the synergistic removal of both divalent cations and anions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yuting Qian,Wenrou Tian,Jun Han,Najun Li,Dongyun Chen,Qingfeng Xu,Hua Li,Jianmei Lu
Catalytic oxidation of HCHO is often limited by the serious recombination of carriers in photocatalysts and the high cost of thermal catalysts based on precious metals. Herein, Bi 4 Ti 3 O 12 nanosheets enriched with bismuth vacancies were synthesized and decorated by UiO-66-NH 2 to obtain VBiTO@NU-66 for efficient removal of HCHO via piezocatalytic oxidation. The Bismuth vacancies in VBiTO enhanced the asymmetry of the crystal structure and introduced the atomic-level channels for energy and electron transfer. After loading UiO-66-NH 2 , the adsorption ability was substantially improved by the formation of Schiff-base covalent bonds between HCHO and –NH 2 . Under the joint action of adsorption and piezocatalysis, piezocatalytic oxidation rate of 300 mg/m 3 HCHO by VBiTO@NU-66 was as high as 95.1% within 3 h, which was 6 times of that of pure BiTO nanosheets. This work offers a novel tactics for the efficient purification of gaseous environmental pollutants.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 41
·93877-93891
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IF 5.8
Zhang Xiaoting,Han Xiaoyu,Liu Yang,Han Runping,Wang Rong,Qu Lingbo
One green adsorbent, UiO-66-NH 2 modified peanut shell (c-PS-MOF), was prepared in a green synthetic route for improving the capture level of aspirin (ASP) and fluoride ion (F – ). The adsorption properties of c-PS-MOF were evaluated by batch experiments and its physicochemical properties were explored by various characterization methods. The results showed that c-PS-MOF exhibited a wide range of pH applications (ASP: 2–10; F – : 3–12) and high salt resistance in the capturing processes of ASP and F – . The unit adsorption capacity of c-PS-MOF was as high as 84.7 mg·g –1 for ASP as pH = 3 and 11.2 mg·g –1 for F – under pH = 6 at 303 K from Langmuir model, respectively. When the solid–liquid ratio was 2 g·L –1 , the content of ASP ( C 0 = 100 mg·L –1 ) and F – ( C 0 = 20 mg·L –1 ) in solution can be reduced to 0.48 mg·L –1 and 1.05 mg·L –1 separately. The recycling of c-PS-MOF can be realized with 5 mmol·L –1 NaOH as eluent. Analysis of simulated water samples showed that c-PS-MOF could be used to remove ASP and F – from actual water. The c-PS-MOF is promising to bind ASP and F – from rivers, lakes, etc. Graphical Abstract
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yicheng Ye,Qiaohong Zhang,Guoying Weng,Zhuwei Zhu,Zhenguo Lyu,Chen Chen
The species and amount of the surface groups are closely related with the catalytic performance for a heterogeneous catalyst. High content of alkylamino (50 mol%) and n -propyl (15 mol%) were simultaneously introduced onto the surface of SiO 2 nanospheres with a one step reverse-phase microemulsion method. Accompanying the formation of plenty of surface nano-bulges, a high ratio (86.5 %) of the silicon species were exposed on the surface of this novel material. Abundant of surface groups including Si-NH 2 (5.5 mmol g −1 ), Si-C 3 H 7 (1.7 mmol g −1 ), and Si-OH (6.1 mmol g −1 ) coexisted on the surface enabled this novel material to be a very efficient catalyst for the Aldol condensation reaction between benzaldehyde and n -heptanal. Higher content of alkylamino supplied more catalytic sites. Proper ratio of silanol-to-alkylamino (a little higher than 1) facilitated the adsorption of the substrate molecules and strengthened the cooperation between alkylamino and silanol. Surface hydrophobic modification with n -propyl further facilitated the adsorption of the substrate molecules at the presence of the byproduct of water. Conversion of 99 % was successfully obtained at a lower temperature (90 °C) and in a very short time of 25 min with the present material being used as the catalyst. In some other Aldol condensation reactions, the present catalyst NH 2 -SiO 2 -C 3 H 7 also showed excellent catalytic performance.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 1
·2283-2297
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IF 5.19
Hu Yuting,Wang Shixing,Zhang Libo,Yang Fan
In wastewater, heavy metal Hg causes serious harm to ecology, so it needs to be removed. In this paper, a novel MOF adsorbent (UiO-66-QU) was prepared by modifying UiO-66-NH 2 with 4-quinolinecarboxaldehyde, which was used to selectively remove Hg(II) from water. The adsorbent was characterized using Fourier transform infrared spectroscopy (FT-IR), field emission scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), zeta potentiometer, and X-ray photoelectron spectroscopy (XPS). In order to investigate the Hg(II) adsorption performance of UiO-66-QU, the effect of time, initial concentration, pH, and temperature were carried out. Langmuir model fitting shows that the maximum adsorption capacity of UiO-66-QU for Hg(II) is 556 mg/g at 298 K. The experimental results show that UiO-66-QU has better Hg(II) adsorption capacity than UiO-66-NH 2 . The isotherm is in accordance with pseudo-second-order models. It is indicated that the adsorption process is mainly monolayer chemical adsorption. The thermodynamic parameters also indicate that the adsorption process is spontaneous and endothermic. It has excellent reusability and selectivity. XPS and the zeta potential showed that the adsorption mechanism was the complex reaction of Hg(II) with nitrogenous group. Therefore, the adsorbent has potential application prospects in removal of Hg(II) from wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Shao-zhong Hu,Ting Huang,Nan Zhang,Yan-zhou Lei,Yong Wang
The discharge of wastewater rich in heavy metals and organic substances has led to the deterioration of the ecosystem, resulting in serious environmental and food pollution, and there is an urgent need to treat the pollutants in the wastewater. Metal organic frameworks (MOFs) have the advantages of large specific surface area and pore volume, as well as the designability of their structures, and are extremely promising materials for wastewater treatment. In this work, a novel adsorbent was synthesized by grafting polyethyleneimine (PEI) onto the UiO-66-NH 2 metal framework (PEI@UiO-66-NH 2 ) via glutaraldehyde-assisted reaction. This new type of adsorbent not only exhibits improved chemical stability in water but also shows greatly increased adsorption sites in comparison with the common UiO-66-NH 2 . The various factors that possibly affect the adsorption behaviors of the PEI@UiO-66-NH 2 were systematically studied. The results show that the PEI@UiO-66-NH 2 can nearly reach the adsorption equilibrium of Pb(II) and methyl orange (MO) within 5 min. The theoretical adsorption capacities toward Pb(II) and MO achieve 692.80 mg/g and 497.51 mg/g, respectively. Specifically, the dynamic theoretical adsorption models were established through the study of the dynamic adsorption of pollutants, providing the theoretical guidance for the scale-up experiments of wastewater treatment with this adsorbent. PEI@UiO-66-NH 2 also shows excellent recycling performance for removing Pb(II) and MO. All these results suggest that PEI@UiO-66-NH 2 has a good application prospect for the removal of wastewater containing Pb(II) and MO.
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Food Analytical Methods
·
2022
·Vol. 15
·期 10
·2830-2839
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IF 3.498
Tang Jing,Li Jie,Liu Tianna,Tang Wenjing,Li Nali,Zheng Shengbiao,Guo Jiahao,Song Changchun
Electrochemical determination of tert-butylhydroquinone (TBHQ) is vital to food safety due to negative health effects; however, bare electrode of traditional electrochemical sensors generally has a narrow linear range and low sensitivity, limiting their practical application. Accordingly, the nano-architecture fabricated with N-doped TiO 2 –carbon nano-composites (TiO 2 /NC) is prepared by the thermolysis of NH 2 functionalized MIL-125(Ti) metal–organic frameworks (NH 2 -MIL-125(Ti)). TiO 2 /NC composites are firstly developed as the electrochemical material for electrochemical determination of TBHQ. The TiO 2 /NC composites with a highly porous structure, excellent conductivity and electron transportation, and large surface area show remarkable electrochemical oxidation ability for TBHQ. Under optimal conditions, TiO 2 /NC composite-modified electrode presents a broader linear response to TBHQ concentration of 0.05–100 μM with the detection limit as low as 4 nM (S/N = 3). Finally, the sensor platform is implemented directly to determine TBHQ in edible oil for evaluation of its practical application. TiO 2 /NC composites sensor fabricated perform larger linear range with high sensitivity and anti-interference properties, which can be used as a potential for electrochemical determination of TBHQ.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jiayou Liu,Xiaoxiang Huang,Linfeng Liu,Qianqian Nie,Zhongchao Tan,Hesheng Yu
UiO-66 variants are widely used for photocatalysis and adsorption, but few studies reported their combined effects in one process. This paper reports that the mechanism behind NO removal using UiO-66-NH 2 includes photocatalytic oxidation and subsequent adsorption. First, the UiO-66-NH 2 was selected out of UiO-66-X variants (X = H, NH 2 , NO 2 , OH, Br, Br 2 ) because of its high NO removal efficiency ( i.e ., 80.54%), which is 8.55–64.95 times higher than those of other UiO-66 variants. Then, the NO reaction pathway and degradation mechanisms are proposed based on the experimental results and theoretical calculations. In an anhydrous environment, the NO removal efficiency increases from 80.54% at 40–60% of humidity to 96.23%. Moreover, NO 2 emissions and catalyst deactivate are not observed. These findings indicate that the photocatalytic NO degradation includes the photocatalytic oxidation of NO into NO 2 on the surface of UiO-66-NH 2 and subsequent NO 2 adsorption in micropores. The reason is that the formation of NO x - ions without H 2 O is theoretically impossible according to the principle of electroneutrality. In-situ DRIFTS also confirms the mechanism. Furthermore, density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulations were carried out to understand the improved NO removal caused by synergistic photocatalysis and adsorption. In summary, this work proposes a new mechanism for NO removal that combines the photocatalytic oxidation and adsorption capability of UiO-66-NH 2 , the new mechanism provides a new strategy to further improve the NO removal efficiency of UiO-66-NH 2 and a new way of inhibiting the deactivation.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Si-Yuan Fang,Ji-Lai Gong,Lin Tang,Wei-Cheng Cao,Juan Li,Zi-Kang Tan,Yu-Wen Wang,Wen-Bo Wang
Thin-film nanocomposite (TFN) membranes with efficient molecular separation and organic solvent resistance are active in demand in wastewater treatment and resource reclamation, meeting the goal of emission peaks and carbon neutrality. In this work, a simple and rational design strategy has been employed to construct a sandwich-structured membrane for removing fluoroquinolone antibiotics and recycling organic solvents. The sandwich-structured membrane is composed of a porous substrate, a hydrophilic tannic acid–polyethyleneimine (TA–PEI) interlayer, and a polyamide (PA) selective layer decorated with metal–organic framework (PA-MOF). Results manifest that the hydrophilic TA–PEI interlayer played a bridging and gutter effect to achieve effective control in amide storage, amine diffusion, and nanomaterial downward leakage at the immiscible interface. The PA-MOF selective layer has been changed to a loosely crumpled surface, endowing functionalities on the sandwich-structured membrane that included limited pores, strengthened electronegativity, and stronger hydrophilicity. Thus, an enhanced water flux of 87.23 ± 7.43 LMH was achieved by the TFN-2 membrane (0.04 mg·mL–1 UiO-66-NH2), which is more than five times that of the thin-film composite membrane (17.46 ± 3.88 LMH). The rejection against norfloxacin, ciprofloxacin, and levofloxacin is 92.94 ± 1.60%, 94.62 ± 1.29%, and 96.92 ± 1.05%, respectively, effectively breaking through the “trade-off” effect between membrane permeability and rejection efficiency. Further antifouling results showed that the sandwich-structured membrane had lower flux decay ratios (3.36∼7.07%) and higher flux recovery ratios (93.40∼98.40%), as well as superior long-term stability after 30 days of filtration. Moreover, organic solvent resistance testing confirms that the sandwich-structured membrane maintained stable solvent flux and better recovery rates in ethanol, acetone, isopropanol, and N,N-dimethylformamide. Detailed nanofiltration mechanism studies revealed that these outstanding performances are based on the joint effect of the TA–PEI interlayer and PA-MOF selective layer, proposing a new perspective to break through the bottleneck of nanofiltration application in a complex environment.
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