SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
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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INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Linzhi Zhai,Xin Zheng,Mengqi Liu,Xinru Wang,Wenli Li,Xiufang Zhu,Aihua Yuan,Yusong Xu,Peng Song
Zr-based metal–organic frameworks (MOFs), especially the UiO-66 family, present a huge application potential for the sorptive eliminations of heavy metal ions, still most of the studies often focus on only one type of adsorbent, thus lacking in some in-depth comparisons on the microstructure produced by the organic ligands. Herein, three kinds of Zr-based MOFs (UiO-66, UiO-66-(OH) 2 , and UiO-66-NH 2 ) are prepared, and their adsorption capacities for Ni 2+ , Fe 3+ and Cr 6+ are systematically investigated and compared. Results suggest that, due to a higher specific surface area of 1569.2 m 2 /g and a larger pore volume of 0.61 cm 3 g −1 , the UiO-66 depicts a better adsorption performance for Ni 2+ and Fe 3+ with larger capacities of 6.8 and 14.1 mg g −1 , respectively. The UiO-66-(OH) 2 presents a specific surface area of 785.5 m 2 /g, which is a little lower than UiO-66 and UiO-66-NH 2 , but shows the maximum adsorption capacity of 39.0 mg g −1 for Cr 6+ , obviously surpassing two other counterparts. In addition, for a multi-ion aqueous solution, UiO-66-(OH) 2 still has an excellent Cr 6+ /Ni 2+ adsorption selectivity of 21.7. The adsorption isotherm of Cr 6+ belongs to monomolecular layer Langmuir model, further verifying –OH 2 + of the UiO-66-(OH) 2 surface acted as the chemical adsorption sites and attracted electronegative Cr 6+ -containing ions. This study dramatically highlights the importance of the organic ligands for MOFs sorbents, which may facilitate achieving their large-scale applications in wastewater treatment.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Guozhi Fan,Yi Chen,Yuchan Lu,Qunpeng Cheng,Bo Chai,Guangsen Song
UiO-66-derived H 2 N-UiO-66-SO 3 H with acid-base active sites was used for the co-production of 5-hydroxymethyl furfural (5-HMF) and furfural (FUR) in the direct conversion of holocellulose composed of cellulose and hemicellulose. The prepared catalyst was further characterized by various techniques, confirming its formation, structure, and composition. H 2 N-UiO-66-SO 3 H displayed excellent performance for the selective conversion of holocellulose to 5-HMF and FUR, achieving yields of 39.1 % and 28.2 %, respectively. The reusability of the catalyst was also investigated by direct use after recycling without any pretreatment. The results indicated that H 2 N-UiO-66-SO 3 H had good stability, and after four cycles, the yields of 5-HMF and FUR decreased only slightly to 37.2 % and 27.1 %, respectively. The recyclable catalyst H 2 N-UiO-66-SO 3 H for the effective conversion of holocellulose to 5-HMF and FUR demonstrated application potential for the utilization of lignocellulosic biomass.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Fangqing Li,Lin Chen,Yufei Wei,Zhiwei Yin,Keying Que
Membrane distillation (MD) is considered an emerging desalination technology. However, the presence of surfactants allows liquid to penetrate the membrane, resulting in membrane wetting, which hinders the commercialization of MD. In this study, we use very few modified materials to prepare novel Janus thin membranes that immobilize modified materials (graphene oxide (GO) and UiO-66-NH 2 ) on polytetrafluoroethylene (PTFE) hydrophobic base membranes via crosslinkers. The composite thin membrane properties with eight different ratios and contents of GO and UiO-66-NH 2 were fabricated and tested by a feed solution of sodium chloride containing a high concentration of sodium dodecyl sulfate. An optimal ratio of Janus membrane with high flux without affecting the effluent water quality was obtained. The Janus membrane exhibited excellent anti-wetting properties compared to the original PTFE membrane. A desalination rate of up to 99.9% was still available even under 48 h of long-term operating conditions by maintaining a flux of approximately 21.2 L/(m 2 ·h). The anti-wetting mechanism of this membrane was further confirmed by the modified XDLVO model. It suggested that the novel Janus membrane could be a highly promising substitute to the MD process for the resource-based treatment of surfactant-containing wastewater, which played an important role in promoting its application.
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MOLECULES
·
2023
·Vol. 28
·期 5
·2182
·
IF 4.6
Panpan Liu,Jiafei Lyu,Peng Bai
In this study, a series of Al-doped metal-organic frameworks (AlxZr(1−x)-UiO-66) were synthesized through a one-step solvothermal method. Various characterization techniques, including X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and N2sorption measurement, suggested that the Al doping was uniform and barely influenced the crystallinity, chemical stability, and thermal stability of the materials. Two cationic dyes, safranine T (ST) and methylene blue (MB), were selected for investigating the adsorption performances of Al-doped UiO-66 materials. Al0.3Zr0.7-UiO-66 exhibited 9.63 and 5.54 times higher adsorption capacities than UiO-66, 498 mg/g and 251 mg/g for ST and MB, respectively. The improved adsorption performance can be attributed to π-π interaction, hydrogen bond, and the coordination between the dye and Al-doped MOF. The pseudo-second-order and Langmuir models explained the adsorption process well, which indicated that the dye adsorption on Al0.3Zr0.7-UiO-66 mostly occurred through chemisorption on homogeneous surfaces. A thermodynamic study indicated the adsorption process was spontaneous and endothermic. The adsorption capacity did not decrease significantly after four cycles.Keywords:metal−organic framework;Al-doped;adsorption;organic dyes;mechanism
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Yang Li,Xiaohuan Zang,Yahuan Li,Shuaihua Zhang,Chun Wang,Zhi Wang
A defective UiO-66 with rich defect sites was synthesized by a modulator-induced defect formation approach and used as the solid-phase microextraction (SPME) fiber coating material. The extraction experimental results showed that the defective UiO-66 coating can selectively extract the fungicides chlorothalonil, vinclozolin, dimethachlon, procymidone and iprodione with a high adsorption capability. The superior adsorption capability can be attributed to hydrophobic, Lewis acid-base and hydrogen bonding interactions. After optimization, a SPME with the defective UiO-66 as the fiber coating combined with GC–MS detection was established for the sensitive and selective determination of the five fungicides in fruit samples. Under the optimized experimental conditions, the quantitative linear response was in the range of 0.83–300 ng g −1 , with the coefficients of determination in the range from 0.9970 to 0.9986 and the limits of detection between 0.25 and 9.0 ng g −1 for the analytes. The method was successfully applied for the determination of the fungicides in different fruit samples. Satisfactory method recoveries (82.7%-117.7%) and good precisions with the relative standard deviations being from 3.2% to 12% were achieved.
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TALANTA
·
2023
·
IF 6.1
Mengyao Mu,Shiping Zhu,Yanmei Gao,Ning Zhang,Youmei Wang,Minghua Lu
Due to widespread application of benzoylurea insecticides (BUs) and its persistence in environment, the effective capture of benzoylurea insecticides residues in environment is an important issue of environmental safety monitoring. To obtain excellent adsorption performance, creating defective structure in metal-organic frameworks (MOFs) can be employed as the method for adjusting its properties. Zirconium(Ⅳ)-based MOF termed as UiO-66-30% was constructed with 2-aminoterephthalic acid (NH 2 -BDC) and terephthalic acid (H 2 BDC) as building blocks. After calcination and removal of thermal-sensitive ligand (NH 2 -BDC), hierarchically porous UiO-66-30% (HP-UiO-66-30%) with multistage pore structure and good stability was obtained. The unique structure of HP-UiO-66-30% endowed it to achieve instantaneous equilibrium (within 2 min) when it was used as a dispersed solid phase extraction (d-SPE) adsorbent to extract BUs from environmental samples, greatly reducing the operation time. A wide linear range (0.05–200 ng mL −1 ), good linearity (R 2 ≥ 0.9980), low detection limits (0.01–0.03 ng mL −1 ) and quantification limits (0.05–0.1 ng mL −1 ) were obtained for BUs. In addition, the HP-UiO-66-30% material possessed the good reusability and the adsorption capacity did not change significantly over 16 adsorption-desorption cycles. Finally, the established dispersed solid phase extraction-high performance liquid chromatography-diode array detector (d-SPE-HPLC-DAD) method was successfully applied to determination of BUs residues in environmental soil samples. The results demonstrated that HP-UiO-66-30% was an excellent sorbent for extraction BUs from environmental samples.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Yalan Wang,Nan Zhang,Danni Chen,Dan Ma,Guoguang Liu,Xuegang Zou,Yuping Chen,Ranjun Shu,Qingyun Song,Wenying Lv
The adsorption behavior and mechanism of Cr(VI) on different acid-modified UiO-66s (Form-UiO-66 and Ac-UiO-66) were systematically investigated for the first time through a series of characterizations, and theoretical calculations of batch experiments. The characterization results demonstrate that acid-modified UiO-66 exhibited a larger specific surface area than did unmodified UiO-66. In addition, since the regulator (formic acid) of Form-UiO-66 was the stronger competition, the specific surface area of Form-UiO-66 (1138 m 2 g −1 ) was larger than that of Ac-UiO-66 (915 m 2 g −1 ). Under optimal experimental conditions, the maximum adsorption capacity of Cr(VI) was 243.9 mg g −1 on Form-UiO-66, and 151.52 mg g −1 on Ac-UiO-66, which was far higher than on the reported unmodified UiO-66 (36.4 mg g −1 ). The results of pH testing, zeta potential, and X-ray photoelectron spectroscopy analysis indicate that Cr(VI) ions were fixed to adsorbent surfaces via electrostatic adsorption. Acid-modified UiO-66 increased the surface active site via the increase in its specific surface area to enhance adsorption capacity of Cr(VI). These results indicated that both the surface charge and specific surface area of the adsorbent primarily determined the Cr(VI) adsorption capacity. Acid modified UiO-66 exhibited enhanced adsorption capacity, stability, and regeneration, compared to traditional adsorbents, and these results provide new insights into adsorption by MOFs.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2019
·Vol. 319
·期 3
·737-748
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IF 1.186
Feng Sheng,Ni Ziqiu,Feng Shanshan,Zhang Zhihui,Liu Shuguang,Wang Runbai,Hu Jiawei
In this study, the UiO-66/Fe 3 O 4 /GO composite was prepared by one step method for removal of cesium ions (Cs + ) in water and exhibited excellent adsorption capacity for Cs + (62.07 mg g −1 ), which can be attributed to the size compatibility of nanosized cavities and the addition of GO. As supporting matrix, GO decreased particle aggregation and increased the surface area of the adsorbent. The composite had good acid and alkali resistance, thermal stability, rapid adsorption rate and can be separated from water by magnetic separation rapidly.
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RSC Advances
·
2019
·Vol. 9
·期 19
·10702-10714
·
IF 3.049
Cunlong Li,Yuqing Zhang,Ming Yong,Wei Liu,Jiaqi Wang
In order to effectively clean oily seawater with anionic polyacrylamide (APAM), UiO-66 coated γ-Al2O3 (UA) composites were firstly synthesized using γ-Al2O3 as a template to induce the growth of high hydrophilic UiO-66 on its surface to form a uniform UA self-assembled membrane. The UA composites and self-assembled membrane were characterized and analyzed. Also, the membrane performance was investigated. The results show that the hydrophilicity of particles is enhanced with the water contact angle decreasing from 39.8° (γ-Al2O3 particles) to 26.2° (UA composites) by introducing the UiO-66 coating. Moreover, the UA self-assembled membrane performs attractive water yield and separation performance. The oil concentration in the permeate treated by the first class of UA self-assembled membrane declines apparently from 91.22 to 18.90 mg L−1, while the water yield is as high as 657.89 L m−2 h−1. The reclaimed separation experiments show that the membrane materials could be recycled by calcination at 200 °C and hydraulic cleaning, which gives the material potential application in cleaning oily seawater.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 31
·15064-15073
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IF 9.931
Xu Jiang,Songwei Li,Shanshan He,Yongping Bai,Lu Shao
Both material choice and filler/organic interface are crucial in mixed matrix membranes (MMMs) for sub-nano-size gas separations and yet, the interface–performance relationship is still a subject of intense debate due to challenging interfacial detection. Herein, two UiO-66-type MOFs (amino-functionalized UiO-66-NH2 and isopropenyl-functionalized UiO-66-MA) are incorporated in cross-linked CO2–philic polyethylene oxide (PEO) matrix based on judicious material screening for CO2 capture. The reactive material UiO-66-MA is stitched together with methacrylate-capped PEO in situ during UV-induced copolymerization to generate highly efficient gas transport passages with conceivably good interfaces. Poor interface is observed by substituting UiO-66-MA with non-reactive UiO-66-NH2 in MPCM (MOF/polymer composite membrane). The interfacial conditions of CO2–philic MPCMs are carefully assessed via advanced physicochemical characterizations for clarifying the correlation between interface and separation performance. The reactive material UiO-66-MA containing MPCM with good interface demonstrates higher gas permeability (up to 1450 barrers) with similar selectivity (up to 45.8 for CO2/N2) when compared to non-reactive UiO-66-NH2 containing MPCM. The mixed gas test also shows high CO2 permeability of 1439 barrer and CO2/N2 selectivity of 37.6 in our MPCM. We also observe unexpected suppressed plasticization/swelling behaviour in UiO-66-MA containing MPCM and enhanced plasticization in UiO-66-NH2 containing MPCM through analysis of gas separation performance in the range of 1–10 atm, which might be utilized as a potential interface assessment tool for nanocomposites. Moreover, the performances of our CO2–philic MPCMs can be optimized further to surpass the (2008) Robeson Upper Bound for highly efficient sustainable CO2 capture.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Sijia Chen,Lin Zhang,Zhao Zhang,Gang Qian,Zongjian Liu,Qun Cui,Haiyan Wang
UiO-66 (UiO for University of Oslo) is a zirconium-based metal–organic framework with reverse shape selectivity, which gives an alternative way to produce high-purity n-heptane (nHEP) used for the manufacture of high-purity pharmaceuticals. A couple of studies have shown that UiO-66 gives a high selectivity on the separation of n-/iso-alkanes. However, the microporous structure of UiO-66 causes poor mass transport during the desorption process. In this work, hierarchical-pore UiO-66 (H-UiO-66) was synthesized and utilized as an adsorbent of nHEP and methyl cyclohexane (MCH) for systematically studying the desorption process of n-/iso-alkanes. A suite of physical methods, including X-ray diffraction patterns, verified the UiO-66 structures, and high-resolution transmission electron microscopy showed the existence of hierarchical pores. N2 adsorption–desorption isotherms further confirmed the size distribution of hierarchical pores in H-UiO-66. Of particular note, the MCH/nHEP selectivity of H-UiO-66 is similar to that of UiO-66 under the same adsorption conditions, and the desorption process of nHEP/MCH from H-UiO-66 is dramatically enhanced; namely, the desorption rates for nHEP/MCH from H-UiO-66 is enhanced by 30%/23% compared with UiO-66 at most. Moreover, desorption activation energy (Ed) derived from temperature-programmed desorption experiments indicate that the Ed for nHEP/MCH is lower on H-UiO-66; that is, the Ed of MCH on H-UiO-66 is ∼37% lower than that on UiO-66 at most, leading to a milder condition for the desorption process. The introduction of hierarchical structures will be applicable for the optimization of the desorption process during separation on porous materials.
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