RSC Advances
·
2020
·Vol. 10
·期 3
·1757-1768
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IF 3.119
Yiqiu Liu,Yi Zhou,Qijun Tang,Qian Li,Si Chen,Zhuxing Sun,Haiqiang Wang
To explore an efficient photocatalyst for NO pollution, a direct Z-scheme photocatalytic system is successfully fabricated by coupling Bi2WO6 with NH2-UiO-66 via a simple hydrothermal synthesis technique. The Z-scheme system promotes the NO photocatalytic oxidation activity with an optimum NO removal rate of 79%, which is 2.7 and 1.2 times that obtained by using only pristine Bi2WO6 and NH2-UiO-66, respectively. Simultaneously, superior selectivity for converting NO to NO3−/NO2− is observed. The enhanced photocatalytic performance of the Bi2WO6/NH2-UiO-66 hybrids is attributed to the following two aspects: (i) large specific area of NH2-UiO-66, which exposes more active sites and is beneficial to the adsorption and activation of NO; (ii) outstanding Z-scheme structure constructed between BiWO6 and NH2-UiO-66, which can improve the efficiency of the separation of electron–hole pairs and preserves the strong oxidation ability of hybrids. ESR analysis shows that ·O2− and ·OH contribute to NO removal. A possible photocatalytic mechanism of NO oxidation on the direct Z-scheme photocatalyst (BWO/2NU) under visible light irradiation is proposed. This work displays the BWO/2NU hybrid's potential for treating low-concentration air pollutants, and the proposed Z-scheme photocatalyst design and promotion mechanism may inspire more rational synthesis of highly efficient photocatalysts for NO removal.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jingcheng Du,Li Chen,Xinjuan Zeng,Shuai Yu,Wei Zhou,Luxi Tan,Lichun Dong,Cailong Zhou,Jiang Cheng
UiO-66 metal–organic frameworks (MOFs) are unstable in some harsh aqueous environments, which limit their practical applications. We demonstrate a postsynthetic modification methodology to transform hydrophilic Zr(Hf)-UiO-66 into superhydrophobic Zr(Hf)-UiO-66-SH-y (SH = thiol, y = fluoroalkyl) by introducing long fluoroalkyl chains into organic linkers through a thiol–ene click reaction. Water contact angles of the four modified UiO-66 MOFs are all larger than 150°. The grafted low-surface-energy fluorine-containing groups become an effective protective shield for the MOFs, making them exhibit remarkable stability in extreme conditions such as alkaline (pH = 12), saturated HCl, and high concentration of NaCl solution (20 wt %). The Zr-UiO-66 MOFs grafted with 1H,1H,2H-perfluoro-1-hexene have high CO2 adsorption contents of 1.54 and 2.88 mmol·g–1 at 298 and 273 K, respectively. Moreover, the superhydrophobic MOFs also showed potential application in oil/water separation.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2019
·
IF 4.978
Jiling Zhao,Chen Wang,Shixing Wang,Yang Zhou
A new adsorbent (MOFs-DHAQ) was prepared by functionalizing UiO-66-NH 2 with 1,8-dihydroxyanthraquinone to remove Pb(II) from wastewater. The optimum pH, adsorption kinetics and adsorption isotherms were studied. MOFs-DHAQ has a good removal rate for Pb(III) at pH 4. It takes only 30 min to reach maximum adsorption capacity about 213.3 mg/g. The experimental data conforms to the pseudo-secondary kinetics and the Freundlich models. The adsorption process belongs to multilayer chemical adsorption . Desorption and adsorption experiments indicate that the adsorbent can be recycled at least four times. The rising temperature favors the adsorption of Pb(II) on MOFs-DHAQ because the adsorption process is a spontaneous endothermic reaction. The interaction mechanism between Pb(II) and the reactive group is mainly electrostatic interaction and complexation. MOFs-DHAQ has excellent selectivity for removing Pb(II) from wastewater contains a variety of interfering ions. The calculated adsorption capacity ( Q ex ) of Pb(II) for column adsorption was 108.04 mg/g and was consistent with the Thomas model's adsorption capacity( Q Th ) about 109.63mg/g. Density functional theory calculations show that MOFs-DHAQ combines with Pb(II) through monodentate N atoms and bidentate O groups. MOFs-DHAQ has good application prospect in the removal of lead from wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Si-Yuan Fang,Peng Zhang,Ji-Lai Gong,Lin Tang,Guang-Ming Zeng,Biao Song,Wei-Cheng Cao,Juan Li,Jun Ye
Metal-organic frameworks (MOFs) materials show great potential in wastewater separation applications. In this study, zirconium-based MOFs (UiO-66) were prepared and constructed universal, high-performance, and flexible nanofiltration (NF) membrane for various dyes and antibiotics separation. The substrate was constructed by two-steps, a) doping graphene oxide (GO) sheets into the membrane casting solution containing polyacrylonitrile (PAN) and forming 2D-3D connecting pores by phase immersion conversion method (defined as GO@PAN), b) immersing the GO@PAN substrate into dopamine solution to self-polymerize into chain macromolecules, which obtaining good compatible and flexible substrate (defined as PGP). Moreover, the UiO-66 was synthesized via solvothermal method and subsequently coated onto the PGP substrate by vacuum-assisted filtration. Benefiting from the water stability, porous structure, and negative charge of UiO-66, the outstanding filtration performance of the UiO-66/PGP thin-film composite (TFC) membrane was achieved. The pure water permeability of the UiO-66/PGP TFC membrane was 31.33 ± 0.75 L m −2 h −1 bar −1 , and the rejection rates for dye (Congo red, Methyl orange, Rhodamine B, and Methylene blue) and antibiotic (Tetracycline hydrochloride, Oxytetracycline, and Ciprofloxacin) were above 94%. Therefore, we further explored the retention mechanism of the UiO-66/PGP TFC membrane for dye and antibiotic separation (size exclusion and electrostatic interaction). More importantly, antifouling properties and long-time stability of the UiO-66/PGP TFC membrane were also evaluated. These results indicated that the prepared UiO-66/PGP TFC membrane is promising for wastewater treatment, separation, and purification in many industrial and pharmaceutical fields.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Guiliang Zhu,Sheng Feng,Jianying Chao,Wei Zheng,Cong Shao
A simple one-pot method was employed to synthesize C-dots modified TiO 2 nanosheets (NS)/UiO-66-NH 2 for enhancing photocatalytic activity. Anatase TiO 2 NS and UiO-66-NH 2 were closely combined and C-dots were well modified on their surfaces. The photocatalytic activities of catalysts were assessed through photodegrading ketoprofen (10 mg/L) under visible light. C-dots/TiO 2 NS/UiO-66-NH 2 degraded 90% of ketoprofen in 80 min, and owned the higher kinetic rate than TiO 2 NS (24 times) or TiO 2 NS/UiO-66-NH 2 (2.1 times). The results indicated that C-dots/TiO 2 NS/UiO-66-NH 2 exhibited the most superb visible-light photocatalytic activity. Besides, C-dots/TiO 2 NS/UiO-66-NH 2 showed good stability and reusability in four runs of degrading ketoprofen. The improved photocatalytic performance was caused by the heterostructure of TiO 2 NS and UiO-66-NH 2 and photoelectrical performance of C-dots, effectively absorbing visible light and promoting photoelectrons transfer.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Xiaohu Ma,Congcong Lv,Peiyu Jiang,Jingbo Geng,Yanli Guo,Yu Zhang,Yuchuan Liu,Yan Jin,Baoxin Li,Wei Liu
The trace acetone determination in breath can be regarded as a noninvasive method for diagnostic of diabetes. There is an urgent demand to develop a simple method for acetone detection which can be easily performed at home. Here, UiO-66-NH 2 @PEI with the appropriate aperture size combined with the hand-held sensor was used to construct the adsorption–desorption sensing platform for separation and enrichment of acetone in exhaled breath (EB). UiO-66-NH 2 @PEI can realize the selective adsorption, desorption and separation for acetone in EB. The flameless combustion hand-held sensor can sensitively respond to acetone in the range of 0.2–12.0 ppm and it can achieve the accurate determination of acetone content in EB of diabetic patients. The hand-held sensor is inexpensive, lightweight and easy to operate, which has great application prospects for the widespread use for diabetic patients in family life.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Fei Wang,Zhe Wang,Junjian Yu,Shuai Han,Xiangwei Li,Yan Wang
Mixed matrix membranes (MMMs) based on metal–organic frameworks (MOFs) are expected to realize efficient separation of CO 2 . However, interfacial compatibility issues between MOFs and polymer matrices limit their performance. In this work, a post-synthesis modification (PSM) strategy was adopted to convert UiO-66 into porous liquids (PLs). MMMs were prepared by incorporating PLs into PIM-1 matrix. The PLs have a liquid-like behavior and can be evenly scattered in PIM-1 matrix to form an interface without defect. The SEM morphology analysis further certified that MMMs had no interface defect and PLs had brilliant compatibility with the polymer film . In addition, the CO 2 -philic ether bonds of the EO fragments enable the MMMs to have superior CO 2 selective separation. Compared with pure PIM-1, the highest CO 2 permeability was improved by 158.0 % and 62.5 % was the increase in CO 2 /N 2 selectivity, arriving at 7211.7 Barrer and 26.0, respectively. Meanwhile, the overall separation performance of MMMs for CO 2 /N 2 exceeds the 2008 Robson upper limit, showing outstanding gas separation performance.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 42
·22859-22867
·
IF 11.9
Jinhong Yang,Haoran Peng,Chong Lin,Qingjiang Pan,Lixue Qi,Li Li,Keying Shi
To overcome the drawbacks of low sensitivity and limited selectivity exhibited by metal oxide sensitive materials, a metal–organic framework (MOF) derived composite (marked as UZZ) was constructed via a combined wet chemical method. UiO-66 was used as the precursor with the introduction of ZnO. The ZrO2 component in UZZ retains the unique octahedral configuration of UiO-66; on its folded surface, a large number of ZnO particles grow, whose sizes range from 20 to 40 nm. The composite exhibits excellent gas sensitivity to NO2 at room temperature. Exemplarily, the gas sensitive response to 100 ppm NO2 is 40.35, with a response time of 1.4 s and a detection limit as low as the 50 ppb level, and the stability is up to 8 weeks. The presence of numerous oxygen vacancies and n–n type heterojunctions on the surface of the UZZ composite synergistically enhances the gas-sensing performance. This finding provides a significant reference for developing new efficient and high-sensitivity metal oxide sensitive materials based on MOFs.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qian Hu,Xuejiao Wang,Yuxuan Zheng,Tianyu Zhao,Jin Qu,Zhong-Zhen Yu,Dongzhi Yang
As chemical warfare agent (CWA) is one of deadly chemicals with strong toxicity and fast action, it is imperative to develop catalytic protective materials that can quickly adsorb and efficiently detoxify CWAs. Herein, reduced graphene oxide (RGO) aerogels are decorated with UiO-66-NCS metal–organic framework with high catalytic activity by in situ growing UiO-66-NH 2 inside the RGO hydrogels, converting the UiO-66-NH 2 to more active UiO-66-NCS, and freeze-drying for realizing solar-thermally enhanced catalytic hydrolysis of dimethyl 4-nitrophenyl phosphate (DMNP), a chemical warfare agent simulant. Compared with UiO-66-NH 2 , the UiO-66-NCS is more efficient in catalytically hydrolyzing DMNP with a 30 % accelerated half-life, and the in situ decoration of the RGO aerogel with UiO-66-NCS further improves the catalytic hydrolysis efficiency because of the more exposed active sites of the UiO-66-NCS. Furthermore, the excellent solar-thermal conversion effect of the RGO porous substrate can rapidly generate heat and transfer it to the UiO-66-NCS catalyst, thereby promoting the catalytic activity of the catalyst. The UiO-66-NCS decorated RGO aerogel exhibits a great detoxification efficiency of DMNP under simulated solar light irradiation with a turnover frequency of as high as 0.0531 s −1 , ∼2.3 times higher than that under room light, and 1.5 times better than that of UiO-66-NCS powder. The solar-thermally enhanced catalytic hydrolysis of DMNP with the UiO-66-NCS decorated RGO aerogel is demonstrated by the quick detoxification of CWA simulant with great recyclability.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Fei Tong,Zan Yang,Zheng Wang,Wenya Liu,Wanqi Jiang,Lu Zhu,Lei Wang,Mingming Zheng,Ruyan Hou,Yibin Zhou,Yingnan Liu
In view of the potential hazards of organophosphorus pesticides (OPs), this paper constructed a ratiometric fluorescent probe utilizing a functionalized metal–organic framework to detect OPs. Ru(bpy) 3 Cl 2 was encapsulated inside UiO-66 as a reference signal, and MnO 2 nanosheets (MnO 2 NSs) were grown on the surface to obtain [email protected] @MnO 2 NSs. Acetylcholinesterase catalyzed the decomposition of acetylcholine into reductive thiocholine, which consumed MnO 2 NSs, thus restoring the [email protected] fluorescence. Due to the enzymatic inhibition of OPs and the redox reaction between MnO 2 NSs and thiamine, this probe emitted blue fluorescence in the presence of OPs. The probe achieved linear responses to dichlorvos and chlorpyrifos with LODs of 9.99 × 10 -6 μg mL −1 and 9.99 × 10 -5 μg mL −1 . The probe exhibited a satisfactory recovery rate for OPs in green tea. Furthermore, a hydrogel detection platform was developed by embedding the probe into sodium alginate. Overall, this work provides a visual approach to detect OPs in agricultural products.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han
Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2 h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 30
·10472-10480
·
IF 4
Pingping Teng,Ying Liu,Zhongqiao Sun,Hao Meng,Yide Han,Xia Zhang
Development of binary MOF-on-MOF heterostructures is a research hotspot in MOFs chemistry due to the advantages elicited by a closely connected interface, which may endow more abundant functionality and even broader applications in interface chemistry. A MOF-on-MOF heterostructure was constructed by in situ growth of MIL-88B on the outer surface of UiO-66. The resultant MIL-88B@UiO-66 produced had an interesting flower-like morphology composed of MIL-88B (petal) on tetrahedral UiO-66 (core). The MIL-88B@UiO-66 heterostructure showed adsorption and Fenton-like oxidation abilities, with distinctly improved structural stability in aqueous solution compared with that of single MIL-88B. Methylene blue (MB) was selected as the target molecule to evaluate the adsorption and Fenton-like oxidation activities. The efficiency of total removal of MB was studied systematically under various operating conditions and the influencing factors were optimized. The kinetics of adsorption and catalytic oxidation were simulated to explore the interactions between MB and MIL-88B@UiO-66. The mechanisms of enhanced adsorption and Fenton-like oxidation were suggested. The cyclic removal performance and structural stability of MIL-88B@UiO-66 were also determined.
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