Membranes
·
2023
·Vol. 13
·期 9
·781
·
IF 4.2
Jiaming Gao,Yongchao Sun,Feifei Kang,Fei Guo,Gaohong He,Hanli Wang,Zhendong Yang,Canghai Ma,Xiaobin Jiang,Wu Xiao
Mixed matrix membranes (MMMs) generally have some fatal defects, such as poor compatibility between the two phases leading to non-selective pores. In this work, PIM-1 was chosen as the polymer matrix, and UiO-66 modified with amidoxime (UiO-66-AO) was used as the filler to prepare the MMMs. In the MMMs, the amino and hydroxyl groups on UO-66-AO form a rich hydrogen bond network with the N and O atoms in the polymer PIM-1 chain to improve the compatibility between the polymer matrix and the filler. In addition, the selective adsorption of CO2by the amidoxime group can promote the transport of CO2in the membrane, which enhances the gas selectivity. The CO2permeability and CO2/N2selectivity of UiO-66-AO@PIM-1 MMMs are increased by 35.2% and 45.2% compared to pure PIM-1 membranes, reaching 7535.5 Barrer and 26.9, surpassing the Robeson Upper Bound (2008) and close to the 2019 Upper Bound. After 38 days of the aging experiment, the CO2permeability is approximately 74% of the original. The results show that the addition of UiO-66-AO has an obvious effect on improving the aging properties of the membrane. The UiO-66-AO@PIM-1 MMMs have a bright prospect for CO2separation in the future.Keywords:amidoxime;UiO-66-AO;mixed matrix membrane;PIM-1;CO2/N2separation
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiuling Zhang,Xiaoke Hao,Zhenyu Zhai,Jiaona Wang,Huiyu Li,Yaxin Sun,Yue Qin,Ben Niu,Congju Li
Wearable electronics based on metal–organic frameworks (MOFs) capable of monitoring various environmental pollutants is a promising approach for realizing gas sensing of chemical information. However, their sensing application combined with electronic textile with breathable, washable and flexible features has not been completely established yet. Herein, we describe a facile and effective strategy to fabricate flexible gas sensor for rapidly detecting hydrogen sulfide (H 2 S) through integrating NO 2 -UiO-66 on electrospun nanofibers membrane (NO 2 -UiO-66 NM) firmly and uniformly. Different from the inherent brittleness and poor processability of powder MOFs, the achieved NO 2 -UiO-66 NM delivers enhanced porosity and surface area, outstanding flexibility, desirable breathability, stable to washing and strong accessibility, more suitable for practical applications. Consequently, the fabricated NO 2 -UiO-66 NM sensor exhibits a significantly high detection selectivity for H 2 S among various analytes (H 2 S, SO 2 , C 6 H 6 , CO and NH 3 ) and remarkable sensitivity for H 2 S with unprecedentedly ultralow detection limit reaching down to 10 ppb. Moreover, the sensing performance can be greatly remained after around five weeks at concentration down to 1 ppm; also, there are slight impact of deformation on sensing activities, revealing superior H 2 S sensing stability. This study offers a feasible solution to develop electronic textiles for chemical sensing application.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Run-dong Ding,Dan-dan Li,Yu-lin Li,Jie-hui Yu,Ming-jun Jia,Ji-qing Xu
Ultrafine and well-dispersed PdAu bimetallic nanoparticles (ca. 1.4 nm) are successfully immobilized on amine-containing UiO-66 frameworks (NH2-UiO-66) via a double-solvent impregnation method. By virtue of the double-solvent strategy, the incorporated PdAu nanoparticles (NPs) are mainly present in the alloy state and distributed inside the cavities of NH2-UiO-66 near the window of the cages. The resulting PdAu/UiO-66 catalysts exhibit much higher catalytic activity and stability for the dehydrogenation of formic acid than the catalyst prepared by the conventional single-solvent impregnation method. The composition-optimized Pd0.8Au0.2/UiO-66-D catalyst affords a very high turnover frequency value of 722 h–1 at 298 K, which is among the highest one in the metal–organic framework-supported Pd-based NP catalysts ever reported under similar reaction conditions. The exceptional catalytic activity and stability of Pd0.8Au0.2/UiO-66-D could be mainly attributed to the formation of highly dispersed PdAu alloy NPs, the suitable electronic structure of Pd species adjusted by the alloy effect, and the metal–support interaction, as well as the abundant amine groups that can promote the activation of the formic acid molecule by forming HCOO– under mild conditions.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Muhammad Zahid,Dongxiang Zhang,Xiyan Xu,Meng Pan,Muhammad Hammad ul haq,Alemtsehay Tesfay Reda,Wenguo Xu
Efficient iodine gas capture is necessitated in many industries like spent nuclear fuel off-gas treatment in view of environmental protection and resource recycling. However, the adsorption efficiency and stability of the current adsorbents are limited. In the present work, efficient and stable barbituric and thiobarbituric acid-based UiO-66-NH 2 adsorbents (i.e., UiO-66-NH-B.D and UiO-66-NH-T.D, respectively) have been synthesized by post-synthetic covalent modification. Characterization approaches, including SEM-EDS, TEM , XRD, FTIR, XPS, 1 H NMR, TGA and BET, are used to obtain information on the properties and adsorption mechanisms of these metal-organic framework (MOF) adsorbents. The kinetics and mechanisms involved are studied in detail. The treatment efficiency and recyclability of the adsorbents are checked and compared with the adsorbents reported in previous works. The results show that the current adsorbents are potentially suitable for efficient iodine gas capture. High maximum iodine adsorption amount by UiO-66-NH-B.D and UiO-66-NH-T.D (1.17 and 1.33 g/g) was achieved under 75 °C. These new adsorbents are thermally stable for iodine adsorption and regenerated and reused with good performance. The adsorption mechanisms were revealed based on experimental results, indicating that iodine is adsorbed by both physisorption and chemisorption .
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Advanced Composites and Hybrid Materials
·
2021
·Vol. 4
·期 3
·562-573
·
IF 5.693
Cheng Xi Quan,Li Songwei,Bao Hongfei,Yang Xiaobin,Li Zhixing,Zhang Yingjie,Wang Kai,Ma Jun,Ullah Asmat,Shao Lu
The lack of highly permeable and selective separation membranes hampers the application of the energy-efficient membrane separation process for water remediation and CO 2 capture in molecular scale. Nanoparticles have been widely applied for tailoring pore structures and surface properties of the molecular separation membranes, thereby enhancing separation performance. However, limited by non-ideal nanoparticle aggregation, it remains a big challenge to fabricate such membranes on a large scale. Herein, we designed a kind of highly dispersed nanoparticles through grafting poly(sodium-p-styrenesulfonate) (PSS) on metal organic frameworks UiO-66 and deployed them for tailoring structure of polyelectrolyte membrane (PEM) for water remediation and Pebax (PEBA) symmetrical membranes for CO 2 capture, respectively. Because of electrostatic interaction, the PSS-grafted-UiO-66 (UiO-66-PSS) demonstrated nearly 100% dispersion in water and had an average particle size around 200 nm. Most interestingly, the introduction of the UiO-66-PSS finely tailored the affinity between membranes and target molecules, and the molecular structure of both PEM and PEBA membranes, thereby tripling the permeances of the membranes and slightly improving the selectivity of the membranes meanwhile. The PEM/UiO-66-PSS membranes demonstrated pure water permeance as high as 27.3 L m −2 h −1 bar −1 with MgSO 4 rejection above 98.7%. For CO 2 capture, the PEBA/UiO-66-PSS membranes exhibited 414.5 barrer with selectivity about 53.8. Taken together, the highly dispersed UiO-66-PSS shows strong promise in constructing molecular separation membranes with high separation performance for environmental remediation. Graphical abstract The highly dispersed PSS-grafted-UiO-66 finely tailored membrane structures of PEM membranes and the PEBA membranes and enhanced affinity between the target molecules and the aforementioned membranes, thereby tripling membrane permeances and improving the membrane selectivity slightly. The obtained PEM/UiO-66-PSS membranes and PEBA/UiO-66-PSS membranes show strong promise in water remediation and CO 2 capture, respectively.
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ANALYTICAL CHEMISTRY
·
2020
·
IF 6.785
Yuqiang Xiang,Huaduo Yan,Bingjie Zheng,Aroosha Faheem,Yonggang Hu
High-throughput analyses of multitarget markers can facilitate rapid and accurate clinical diagnosis. Suspension array assays, a flow cytometry-based analysis technology, are among some of the most promising multicomponent analysis methods for clinical diagnostics and research purposes. These assays are appropriate for examining low-volume, complex samples having trace amounts of analytes due to superior elimination of background. Physical shape is an important and promising code system, which uses a set of visually distinct patterns to identify different assay particles. Here, we presented a morphology recognizable suspension arrays based on the microorganisms with different morphologies. In this study, UiO-66-NH2 (UiO stands for University of Oslo) metal–organic frameworks (MOFs), was wrapped on the microorganism surface to form an innovative class of microorganism@UiO-66-NH2 composites for suspension array assays. The use of microorganisms endowed composites barcoding ability with their different morphology and size. Meanwhile, the UiO-66-NH2 provided a stable rigid shell, large specific surface area, and metal(IV) ions with multiple binding sites, which could simplify the protein immobilization procedure and enhance detection sensitivity. With this method, simultaneous detection of three colorectal cancer-related microRNA (miRNA), including miRNA-21, miRNA-17, and miRNA-182, could be easily achieved with femtomolar sensitivity by using a commercial flow cytometer. The synergy between microorganisms and MOFs make the composites a prospective barcoding candidate with excellent characteristics for multicomponent analysis, offering great potential for the development of high throughput and accurate diagnostics.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Fukun Bi,Xiaodong Zhang,Shang Xiang,Yunyun Wang
The effect of Pd loading (0.25, 0.5 and 1.0 wt%) and ZrO 2 support calcined at diverse temperatures (600, 700 and 800 °C) by pyrolysis of UiO-66 was investigated for CO oxidation in this work, respectively. The physicochemical properties of the samples were characterized by various characterization methods. The XRD results exhibited that all ZrO 2 support possessed mixed crystalline phase, the monoclinic ZrO 2 and tetragonal ZrO 2 . And the calcination temperature had a big impact on the composition of ZrO 2 supports. Pyrolysis of UiO-66 at high temperature was favorable for the formation of monoclinic ZrO 2 . Additionally, the introduction of Pd was induced the phase conversion from tetragonal to monoclinic of ZrO 2 . The order of catalytic efficiency was as follows: 0.5Pd/Zr-700 > 0.5Pd/Zr-600 > 0.5Pd/Zr-800. Moreover, 0.5Pd/Zr-700 presented high stability and great reusability. The good catalytic performance of 0.5Pd/Zr-700 was ascribed to the better reduction ability at low temperature and high O ads /O lat and Pd 0 /Pd 2+ on the surface. Importantly, the reaction pathway of CO oxidation over the 0.5Pd/Zr-700 was exposed.
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INORGANICA CHIMICA ACTA
·
2020
·
IF 2.304
Xue Dong,Yongcen Lin,Yuqin Ma,Lang Zhao
A post-synthetic approach using nitrogen-containing substances modify UiO-67 was proposed to enhance its adsorption for Congo red (CR). The newly synthesized materials were thoroughly analyzed by SEM, TEM, EDX, XPS, XRD, FT-IR, TGA and BET techniques. Results showed that N was successfully incorporated into UiO-67 frameworks to prepare of N X -UiO-67, through coordination interaction with Zr-O clusters. Compared to parent UiO-67, the obtained N X -UiO-67 exhibited a significant increase in adsorption of CR, and the adsorption capacities for CR were in the following order: N U -UiO-67 (2360 mg g −1 ) > N T -UiO-67 (1986.3 mg g −1 ) > N A -UiO-67 (1493 mg g −1 ). Moreover, the pseudo-second-order kinetics and the Langmuir isothermal model exhibited a better fit to describe the adsorption behavior of CR onto the N X -UiO-67.
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MOLECULES
·
2021
·Vol. 26
·期 19
·5736
·
IF 4.412
Chunhua Wang,Zhiquan Yu,Yuhao Yang,Zhichao Sun,Yao Wang,Chuan Shi,Ying-Ya Liu,Anjie Wang,Karen Leus,Pascal Van Der Voort
Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2reduction. The obtained Pd/UiO-66-NO2catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.Keywords:Pd/UiO-66-NO2;furfural;hydrogenative ring-rearrangement;cyclopentanone;double-solvent method
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2019
·Vol. 319
·期 3
·737-748
·
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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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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