MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2024
·
IF 4.2
Z.H.A.O.-X.U.A.N. Jiang
In this investigation, UiO-66-NH 2 was effectively synthesized through a solvothermal approach, utilizing benzoic acid and hydrochloric acid (HCl) as modulating agents. This synthesis process intentionally introduced defects mediated by benzoic acid, and the degree of these defects was precisely adjusted by the concentration of HCl. Subsequently, the material underwent a covalent modification process through an amidation reaction, resulting in the attachment of tetrakis (4-carboxyphenyl) porphyrin (TCPP). The results demonstrated a significant improvement in the photocatalytic reduction of Cr(VI), showcasing a 125 % elevation in reduction efficiency as compared to the unmodified UiO-66-NH 2 material serving as the baseline. The performance enhancement is due to the synergistic effect of the defect structure and TCPP modification, which enhances the light absorption, promotes charge transfer and separation, reduces the recombination rate, and improves the adsorption capacity and light absorption efficiency of Cr(VI). This research introduces an innovative approach and a highly effective catalyst, offering a novel solution for modifying metal-organic frameworks (MOFs) and enhancing their photocatalytic performance in the reduction of Cr(VI).
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DALTON TRANSACTIONS
·
2024
·
IF 3.5
Zhengyan Wang,Chenhao Yuan,Dong Yang,Mifen Cui,Jihai Tang,Zhuxiu Zhang,Xu Qiao
It is of great significance to develop catalysts for the degradation of hexachlorobenzene from the industrial thermal process. In this paper, formic acid was used as a modulator to generate defect sites in Ce/Zr-UiO-66 with intrinsic Brønsted acidity. The defective formate ligands were removed through methanol–water vapor treatment to expose additional open metal sites with Lewis acidity. The intrinsic Brønsted acid sites of the resulting Ce/Zr-UiO-66-FA-P achieved a hexachlorobenzene degradation efficiency of 99.5% at 250 °C. The generated Lewis acid sites facilitated the C–C cleavage of degradation intermediates. More than 95.0% of the final products were CO2/CO, coupled with chlorinated alkanes/alkenes, which outperformed other benchmark metal oxide catalysts. The Ce/Zr-UiO-66-FA-P catalyst maintained its catalytic activity in the model industrial flue gas and humid environment. The degradation pathway of hexachlorobenzene was tracked using in situ FT-IR spectra.
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MOLECULES
·
2025
·Vol. 30
·期 7
·1487
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IF 4.6
Senliang Xi,Dawei Xu,Renzeng Chen,Wenhao Yao,Wenying Wu,Teng Zhang,Liang Yu
Ammonia borane (AB) has attracted much attention in the field of solid-state hydrogen storage due to its high hydrogen storage capacity. Nanoconfinement in UiO-66 can reduce the hydrogen release temperature. In particular, terephthalic acid was used as a linker to further improve the dehydrogenation properties through the modification of -NH2, -OH, -NO2, -Br, and -F groups. The hydrogen release content of 0.5AB/UiO-66 was 1.98 wt.%, whereas the hydrogen release content of UiO-66-2OH modified by -OH groups increased to 3.85 wt.%. The non-covalent interaction results show that -NH2and -OH preferred adsorption with -BH3, and the H in -NH2and -OH were able to interact directly with the H in AB to modify the dehydrogenation process of AB, whereas -NO2, -Br, and -F indirectly affected the charge density of hydrogen atoms in AB to alter the dehydrogenation property of AB. The modification of functional groups provides a theoretical basis for the design of high-performance MOF nanoconfinement AB composite hydrogen storage materials.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
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IF 7.7
Xiaoyao Wang,Haizhi Huang,Siyao Zhong,Xuping Shentu,Zihong Ye,Xiaoping Yu
Fenpropathrin residues in grain are potentially harmful to humans. Therefore, a fluorimetric lateral flow immunoassay using a zirconium-based organic skeleton (UiO-66) as a signal marker was developed for detecting fenpropathrin. Herein, carboxymethyl chitosan (CMCS) was used to modify UiO-66 and improve its water solubility to facilitate stable binding with sodium fluorescein (NaFL). This resulted in formation of a new fluorescent probe that is more suitable for lateral flow immunoassay (LFIA). The materials were characterized via electron microscopy , Fourier-transform infrared spectroscopy, and powder X-ray diffraction. CMCS and NaFL were successfully bound to UiO-66. Under optimized conditions, the constructed NaFL/UiO-66@CMCS-LFIA exhibited a good linear relationship within the range of 0.98–62.5 μg/L, with a detection limit of 3.91 μg/L. This probe was fourfold more sensitive than traditional colloidal gold nanoparticle-based LFIA. Finally, NaFL/UiO-66@CMCS-LFIA was successfully applied to detect fenpropathrin in wheat and maize samples. The detection limit was 1.56 μg/kg and recoveries ranged from 96.58 % to 118.56 %. This study provides a sensitive, stable, and convenient method for the rapid detection of pesticide residues .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuchen Cui,Xiaolei Cui,Lubomira Tosheva,Chunzheng Wang,Yongming Chai,Zixi Kang,Qiang Gao,Kun Wang,Zhihan Zhang,Hailing Guo,Daohong Xia,Daofeng Sun
Effective separation of CO 2 from CH 4 is crucial for the purification of natural gas, which requires membrane materials with high permeability, selectivity, and stability of under high pressures. In this work, a high CO 2 -affinity MOF-based nanofiller (P in @NH 2 -UiO-66) was prepared and integrated in polyetherimide (PEI) to prepare mixed matrix membranes (MMMs) for enhanced CO 2 /CH 4 separation capabilities. The P in @NH 2 -UiO-66 nanofiller comprised an in situ-formed polyethyleneimine-NH 2 -UiO-66 composite prepared via a one-pot synthesis. The polyethyleneimine was covalently attached to the H 2 BDC-NH 2 ligand allowing for a stronger integration within the PEI matrix. The polyethyleneimine affects the nucleation of MOF, leading to miniaturization of the MOF particles. The smaller-sized filler is beneficial for improved interaction at the filler-matrix interface. The numerous amino functionalities grafted onto the NH 2 -UiO-66 increased the CO 2 adsorption sites, thereby enhancing the affinity for CO 2 . Owing to the improved interaction, the elevated CO 2 attraction, and the inherent properties of the porous NH 2 -UiO-66, the fabricated MMMs preformed superior in separating CO 2 /CH 4 . The 30-P in @NH 2 -UiO-66-PEI membrane (containing 30 wt% nanofiller) exhibited a CO 2 /CH 4 selectivity of 27.7 and a CO 2 permeability of 2498.9 Barrer. The CO 2 permeability was 21 times greater than that of the pristine PEI membrane, and 4 times higher compared to P@NH 2 -UiO-66 MMM with polyethyleneimine modified MOF filler prepared by a traditional wet impregnation method. Additionally, the novel MMM demonstrates excellent separation stability under conditions that mimic industrial settings, demonstrating its potential application for natural gas purification.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2025
·
IF 4.7
Yanhao Xu,Ziyi Zhong,Pinle Zhang,Huancheng Huang,Kuan Cai,Xinliang Liu
Persistent organic pollutants (POPs) represent a significant environmental and health risk due to their high toxicity, persistence, strong accumulation potential, and adverse effects on human health. 4-Chlorophenol (4-CP), a type of POP, has low catalytic efficiency at low concentrations and is easily interfered with by other pollutants, making its degradation challenging. A new “recognition-enrichment-in-situ degradation” strategy is introduced to selectively remove chlorophenols from contaminated aqueous environments. In this study, ionic liquids were incorporated into the UIO-66 framework as active sites for selective adsorption. 4-CP contains phenolic hydroxyl groups and exhibits high polarity. The dispersive interactions between 4-CP and ionic liquids, along with hydrogen-bonding interactions between the Tf 2 N anion and the hydroxyl groups of 4-CP, enhance the selective enrichment of 4-CP within the nanocavities of the metal–organic frameworks (MOFs). Fe 3+ was then introduced, enabling in-situ degradation of 4-CP through photo-induced generation of free radicals and cavities from H 2 O 2 catalyzed by Fe-IL@UIO-66. The results indicated that the adsorption capacity of IL@UIO-66 for 4-CP reached 53 %, significantly higher than that for five other organic pollutants. The adsorption capacity of IL@UIO-66 for 4-CP reached 509.5 mg g −1 , 49.9 % greater than that of the original UIO-66. The degradation efficiency of 4-CP by Fe-IL@UIO-66 increased from 61 % to 81 %, and after four cycles, the material retained a catalytic activity with a degradation efficiency of 64.2 %. This study provides valuable insights into the recognition-enrichment-in-situ catalytic strategy for treating low-concentration, highly toxic wastewater.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Wei Zhao,Hongjing Liu,Chengpeng Zhang,Yuyang Cao,Yuying Xu,Xueli Liu,Zhen Lu
Metal–organic frame UiO-66-NH 2 was modified by 3-glycidyl ether oxypropyl trimethoxysilane (KH560), and KH560-UiO-66-NH 2 was synthetized and added to Pebax to prepare KH560-UiO-66-NH 2 /Pebax mixed matrix membranes (MMMs). The epoxy group of KH560 had an amine-epoxidation reaction with the NH 2 in UiO-66-NH 2 , which prevented UiO-66-NH 2 from agglutinating in the MMMs. In addition, the N H bond and OH bond of KH560-UiO-66-NH 2 could theoretically form hydrogen bonds with CO and N H bonds in the main chain of polymerization, respectively, so as to improve the interfacial compatibility between fillers and polymers. The structure and properties of the filler particles and MMMs were evaluated by Fourier transform infrared spectrometer, x-ray diffraction, scanning electron microscopy, and thermogravimetric analyzer. The results showed that the filler particles were successfully synthesized, and had good crystallinity, uniform size distribution, and good thermal stability. The inorganic and organic interfaces of MMMs had no obvious interface defects. The obtained KH560-UiO-66-NH 2 /Pebax MMMs showed CO 2 permeability of 111.52 Barre and CO 2 /N 2 selectivity of 92.16, which were 85.65% and 88.73% higher than that of pristine membranes, respectively. The gas separation performance of MMMs was significantly improved, exceeding the upper bound of 2008 Robeson.
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Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
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高影响因子
RARE METALS
·
2024
·
IF 9.6
Liu Cheng,Shi Ying-Zhang,Chen Qi,Ye Bing-Hua,Bi Jin-Hong,Yu Jimmy C.,Wu Ling
Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce 3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H–N···Ce and the C–S···Ce interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O 2 activation and reduction occur at coordinatively unsaturated Ce 3+ sites to form ·O 2 – . This is accelerated by the Ce 3+ /Ce 4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level. Graphical abstract
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wenmin Li,Tingting Xu,Fangmeng Sheng,Yue Wang,Yifan Li,Yuan Xia,Bin Wu,Xingya Li,Tongwen Xu
The selective separation of monovalent ions remains a challenge because of the similar sub-nanometer sizes. Metal-organic frameworks (MOFs) are promising candidate membranes for ion selective separation based on the angstrom sized windows for size sieving. Here, to further enhance the monovalent ion selectivity , 1, 5-naphthalenedisulfonic acid tetrahydrate (NTDS) molecules with sulfonate groups are incorporated to offer a binding affinity, generating a UiO-66@NTDS membrane via the window-cavity structure confinement. In addition to the size sieving effect, the charge and affinity interaction can compensate the energy loss induced by the ion dehydration. Thus, the UiO-66@NTDS membranes exhibit elevated separation performance compared to the original UiO-66 membranes under the concentration gradient driven, accompanied by high monovalent cation permeation rates (i.e., 0.3–0.7 mol m −2 h −1 ) and mono-/divalent cation selectivities (i.e., ∼73 for K + /Mg 2+ , ∼57 for Na + /Mg 2+ , and ∼46 for Li + /Mg 2+ ). This work provides guidelines for the development of efficient ion-selective MOF membranes via the combination of size sieving and interaction attraction.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Chengli Jiao,Xiangju Song,Xiaoqian Zhang,Lixian Sun,Heqing Jiang
Control of the surface morphology of polyamide membranes fabricated by interfacial polymerization is of great importance in dictating the separation performance. Herein, polyamide membranes with a specific nanoscale striped Turing structure are generated through facile addition of Zr-based metal–organic framework UiO-66-NH2 in the aqueous triethylenetetramine phase. Interestingly, accompanied by the degradation of UiO-66-NH2 in aqueous solution, an intermediate complex is in situ formed through the strong interaction between the Zr metal center and the amine group from triethylenetetramine, which can lower amine diffusion and induce a local interfacial reaction, contributing to the generation of a homogeneous nanoscale striped Turing structure. The resulting membranes are used for CO2/CH4 gas separation. Compared with the parent polyamide membrane displaying a CO2/CH4 selectivity of 43.1 and a CO2 permeance of 31.5 GPU, the membrane with 0.02 wt % of UiO-66-NH2 introduced into the aqueous phase shows a higher CO2/CH4 selectivity of 58.3, along with a CO2 permeance of 27.1 GPU. Additionally, when 0.1 wt % of UiO-66-NH2 is incorporated into the aqueous phase, the membrane exhibits a combination of a higher CO2/CH4 selectivity and an enhanced CO2 permeance in contrast with the parent polyamide membrane.
研究领域:
材料科学
·
化学工程
·
环境科学
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yinghui Xu,Xuan Zhao,Ran Chang,Hongqiang Qu,Jianzhong Xu,Jing Ma
Rationally regulating the separation pores is an effective way to achieve efficient separation membrane . However, the developed metal-organic framework (MOF) membranes for water treatment are all formed by one kind of MOF, which can only provide rigid pores, makes it difficult to achieve high flux and excellent rejection ratio simultaneity. Here, we proposed a facile strategy for the synthesis of heterogeneous MOF-on-MOF membrane with hierarchical pores, by site-specific grown ZIF-8 layer on UiO-66-NH 2 layer. Thus unique architecture of the obtained double-layered MOF membrane (UiO-66-NH 2 @ZIF-8) endows multidimensional separation pores: (i) the large pores of UiO-66-NH 2 can facilitate water transportation, (ii) the molecular-sieving pores of ZIF-8 can intercept dyes, (iii) UiO-66-NH 2 acting as active sites can promote the growth of ZIF-8. As a result, the optimized UiO-66-NH 2 @ZIF-8 membrane exhibits high flux (36.7 L m −2 h −1 bar −1 ) and excellent dye rejections (>97.0%). Through analysis and comparison, the regulated multi-type pores play an important role in membrane performance. Coupled with the facile membrane preparing method, this work can used as a potential approach of designing other advanced MOF membrane for water treatment.
研究领域:
材料科学
·
环境工程
·
化学工程
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