Journal of Cleaner Production
·
2023
·
IF 11.1
Di Zhang,Hao Tang,Bing Zhao,Lijie Liu,Hongwei Pang,Xiangxue Wang,Shujun Yu
Radioactive uranium removal plays a key role in energy development and environmental security. Sulfide nanoscale zero-valent iron (S-NZVI) has good antioxidant capacity, dispersibility and activity to eliminate U(VI) from wastewater, but the removal efficiency is limited. To improve the reduction and adsorption capacity of S-NZVI, through treating Fe 3+ solution by nitro-functionalized UiO-66 (UiO-66-NO 2 ) with high porosity, UiO-66-NO 2 enhanced S-NZVI adsorbent (S-NZVI/UiO-66) was prepared by liquid phase reduction method. The smaller size and larger specific surface area of S-NZVI/UiO-66 were confirmed by a variety of characterization techniques. Based on the excellent surface structure and reactivity, the U(VI) removal capacity of S-NZVI/UiO-66 (895 mg g −1 ) was much better than S-NZVI (434 mg g −1 ) and UiO-66-NO 2 (267 mg g −1 ). The impacts of pH, background ion strength, coexisting ions and different water environments on adsorption were studied via macroscopic batch experiments. The results showed that S-NZVI/UiO-66 could remove U(VI) adequately in a wide pH range. The removal rate was basically not affected by the concentration of NaNO 3 , demonstrating that the adsorption process of U(VI) on S-NZVI/UiO-66 tended to inner surface complexation. From XPS technique combined with the results of batch adsorption experiments, it was clear that the elimination mechanisms of U(VI) by S-NZVI/UiO-66 were mainly the physical adsorption, electrostatic attraction and complexation of UiO-66-NO 2 , and the reduction and complexation of S-NZVI. Therefore, it is believed that S-NZVI/UiO-66 has a great potential to be an excellent adsorbent in the field of the environment remediation. Moreover, S-NZVI/UiO-66 promises to be a novel nanomaterial for solving the problem of radionuclide contamination in practical environments.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Shanshan Zeng,Fucong Lyu,Ligang Sun,Yawen Zhan,Fei-Xiang Ma,Jian Lu,Yang Yang Li
In this work, UiO-66-based metal–organic frameworks are investigated as an oxygen reduction reaction (ORR) catalyst for the first time. UiO-66-NO2 is solvothermally grown on the surface of cobalt phthalocyanine-anchored carbon nanotube (CoCNT) surface, serving as an oxygen “pump” to accelerate the oxygen reduction reaction (ORR). The UiO-66-NO2-attached CoCNT (UiO-66-NO2@CoCNT) exhibits superior electrochemical catalytic properties, exceeding the state-of-the-art commercial 20% Pt/C catalyst with more positive half-wave potential (15 mV difference, at 1600 rpm), better stability (no significant degradation for UiO-66-NO2@CoCNT vs 19% degradation for 20% Pt/C after 25 000 s), and higher methanol tolerance. When assembled in a flexible zinc–air battery, the UiO-66-NO2@CoCNT remains a competitive alternative to commercial 20% Pt/C catalyst with comparable power density and excellent flexibility, suggesting its potential in wearable electronic devices. The outstanding performance of UiO-66-NO2@CoCNT composite is closely related to the synergetic effect among the three components: CNT as a conductive backbone, cobalt phthalocyanines as the oxygen reduction catalytic active site, and UiO-66-NO2 as an ideal oxygen adsorption pump (the oxygen diffusion rate is 4.8 times that of 20% Pt/C and 17.7 times that of CoCNT). The synergy between the three components facilitates oxygen adsorption, transfer of adsorbed oxygen molecules, oxygen reduction, and electron conduction.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
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
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2022
·Vol. 194
·期 11
·5167-5184
·
IF 3.094
An Peide,Zhu Fenfen,Liu Shiji,Zhou Xiaolin,Wang Chunfang,Liu Yufeng,Meng Hao,Zhang Xia
Recently, metal–organic frameworks (MOFs) are considered to be the moderate hosts for the bio-enzymes owing to their unique 3D pores and controllable surface affinity to the target molecules. In this work, the benzoic acid (BA)–modulated UiO-66-NO 2 was introduced, and cytochrome c (Cyt C) was chosen as the target enzyme to evaluate the immobilization efficiency of the resulting UiO-66-NO 2 -BA. The immobilization conditions including pH, adsorption time, and temperature and the initial concentrations of BA were optimized. The adsorption kinetics and thermodynamics were analyzed to further explore the enhanced adsorption mechanism. It is worth noted that all the UiO-66-NO 2 -BA exhibited evidently enhanced adsorption capacities in comparison with the unmodified UiO-66-NO 2 due to the formation of the chemical bonds between the UiO-66-NO 2 -BA and cytochrome C, indicating the positive roles of BA modification. Finally, the activities of the immobilized cytochrome C were assessed by using the catalytic oxidation of ABTS in the presence of H 2 O 2 , which reactions were also conducted over the free cytochrome C for comparison. The evidently improved stability under definite pH range, prolonged durability against the organic solvents, and the good reusability of the immobilized cytochrome C highlight the prospect applications of functional MOF immobilized enzymes in the practical catalytic reactions. Graphical abstract
研究领域:
生物化学
·
材料科学
·
酶工程
✓ 已验证
DOI
高影响因子
FOOD CONTROL
·
2021
·
IF 5.548
Weixia Yang,Jinmeng Wang,Yong Han,Xueli Luo,Wenzhi Tang,Tianli Yue,Zhonghong Li
Pb(II), a highly toxic heavy metals that targets the human nervous system, has contaminated water and food in recent years. The nanomaterial of Metal–organic frameworks (MOFs) possesses superior removal performances. However, their practical application is limited by their nature of fine powdery. Herein, we developed robust MOFs film without the adding of polymer in MOFs ink and the modification of the substrate, which was achieved by choosing appropriate substrate of gelatin hydrogel with functional groups and simple thermal-treatment after coating UiO-66-NO 2 onto gelatin hydrogel. The volatilization of the UiO-66-NO 2 dispersant ethyl acetate promotes the rearrangement and dense accumulation of UiO-66-NO 2 crystals to form a dense UiO-66-NO 2 film. During the following thermal-treatment process, –COOH of UiO-66-NO 2 and –NH 2 of gelatin chemically reacted to establish the stable composites of UiO-66-NO 2 film and gelatin hydrogel. The results of batch adsorption experiments demonstrate that adsorption behaviors of the as-synthesized gelatin/UiO-66-NO 2 film composite hydrogels can be explained by the pseudo-second-order kinetic model and the Langmuir isotherm model, stating that this adsorption process involves with a chemical monolayer adsorption. Besides, gelatin/UiO-66-NO 2 film composite hydrogels own satisfactory removal efficiency for Pb(II) in apple juice, and the adsorption process has little impairment on the quality of apple juice. These results suggest that MOFs film is suitable for water decontamination and food safety control fields.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Xiao Ling,Xiaofeng Guo,Ke Wang,Ziming Huang,Zhixuan Mo,Huibo Qin,Linhai Duan,Xiuhong Meng,Hui Wang
Photocatalytic degradation of organic pollutants in water represents a highly promising strategy for environmental remediation. However, conventional photocatalysts are hampered by their inefficient employment of visible light energy and the propensity of photoinduced charge carriers to undergo recombination. To overcome these limitations, Z-scheme photocatalyst UiO-66-NO 2 @ Ag/AgCl (UiO@Ag-X, where X denotes the Ag/AgCl content) composites were designed and prepared. The crystal structure, morphology, photocatalytic performance, light absorption capacity, and carrier separation efficiency were systematically tested. Optical and electrochemical measurements revealed that the incorporation of Ag/AgCl enhanced the segregation and transfer efficiency of charge, which is crucial for boosting photocatalytic activity. These improvements directly contributed to the enhanced degradation efficiency observed in subsequent experiments. In experiments using methyl violet (MV) as the model pollutant, the photocatalytic degradation performance of UiO@Ag-X samples was evaluated. Among these samples, UiO@Ag-50 achieved a remarkable degradation efficiency under light irradiation. Moreover, the corresponding kinetic rate constant was about 0.04724 min -1 , which was higher than that of UiO-66-NO 2 . Quenching experiments were employed to investigate the mechanisms related to photocatalysis. The results show that hydroxyl radicals play an important role in the degradation of MV.
研究领域:
环境科学
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Zixu Wang,Linna Han,Qing Xia,Wanfang Feng,Songtao Li,Liyan Liu
Enrichment and quantification of sugar phosphates (SPx) in biological samples are of great significance in biological medicine. In this work, a magnetic nanoscale metal–organic framework composite, Fe3O4@UiO-66-NO2, was synthesized and utilized as a high-capacity adsorbent for the enrichment of SPx in biological samples. Fe3O4@UiO-66-NO2 exhibited a high specific surface area (310.02 m2/g), a suitable pore size (3.47 nm), and strong magnetism (14.99 emu/g), enabling convenient separation and recovery. Experimental results demonstrated that Fe3O4@UiO-66-NO2 exhibited excellent adsorption performance for five types of SPx, achieving complete adsorption within 6 min at a dosage of 200 μg, and the adsorption process exhibited pH tolerance. The adsorption isotherm result indicated that the maximum adsorption capacities for different SPx ranged from 234.06 mg/g to 403.24 mg/g. Adsorption mechanisms using X-ray photoelectron spectroscopy, FT-IR, and density functional theory revealed multiple interactions, such as coordination and hydrogen bonding, and contributed to the adsorption process. A magnetic nanoscale-dispersive solid-phase extraction protocol was developed based on a Fe3O4@UiO-66-NO2 for rapidly enriching SPx from biological samples. The protocol allowed for SPx detection over a wide linear concentration range, low limits of detection (0.001–0.02 ng/mL), high precision (<7.88%), and good accuracy (82.56%–119.66%). This protocol was successfully applied to real blood samples, prefiguring the great potential of magnetic MOFs for the enrichment and detection of SPx in biological samples.
研究领域:
分析化学
·
材料科学
·
纳米技术
·
生物化学
·
环境科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xianjie Wang,Yaning Zhao,Hengsheng Wei,Yi Wang,Jingdong Gou,Jinhui He,Xue Ma,Louwei Cui,Liuyi Pan,Jiaojiao Liu,Dong Li
The separation of coal-derived C8 cyclohexane isomers, particularly cis-1,3-dimethylcyclohexane (cis-1,3-DMCH) and ethylcyclohexane (ECH), remains challenging due to their similar molecular structures and physicochemical properties, while research on cycloalkane isomer separation is limited. A series of functionalized UiO-66 derivatives (UiO-66, UiO-66-(CH 3 ) 2 , UiO-66-OH, and UiO-66-NO 2 ) were synthesized via solvothermal methods and systematically evaluated for their adsorption and separation performance toward C8 cyclohexane isomers through single-component and competitive batch adsorption experiments, dynamic breakthrough tests, and molecular simulations. Among the investigated materials, UiO-66-NO 2 demonstrated superior selectivity (α = 5.10) for cis-1,3-DMCH over ECH, with excellent regeneration stability over multiple cycles, significantly outperforming commercial activated carbons and zeolites. Mechanistic studies revealed that the enhanced selectivity arises from a dual mechanism combining geometric confinement effects and electronic recognition, where the oblate geometry and larger dipole moment of cis-1,3-DMCH enable preferential adsorption through strengthened C-H···O and C-H···NO 2 interactions, as confirmed by calculated binding energies (−37.15 kJ/mol for cis-1,3-DMCH vs. -22.13 kJ/mol for ECH) and diffusion coefficients. This work demonstrates rational MOF functionalization for efficient cycloalkane isomer separation, providing a promising strategy for coal-derived naphtha valorization.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 3.7
Zhaorui Qi,Xurui Li,Yueming Zhu,Li Li,Yu Liu
Metal–organic framework (MOF) is a porous material composed of metal ions/clusters and organic ligands. It has attracted much attention due to its high specific surface area, good biocompatibility, chemical modifiability, and diversity of components. Among many MOFs, zirconium-based MOFs are particularly suitable for biological applications due to their optimal stability and low toxicity to hydrolysis. However, due to the weak coordination bonds between many metal clusters and organic ligands, most MOFs are prone to collapse in acidic environments, and the stability of MOFs as drug carriers cannot be guaranteed so that they cannot be widely used as oral drug carriers. This study synthesized the three MOFs using metal Zr ion clusters as the center and different nitrogen-containing organic ligands, which are stable in gastric acid, namely, UiO-66-PDC, UiO-66-NH 2 , and UiO-66-NO 2 . The anionic drug loxoprofen (LOX) was loaded and characterized using scanning electron microscopy, infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, and x-ray diffraction. The adsorption and release behaviors of LOX and the three MOFs were studied from the molecular point of view by computer simulation. A series of behaviors and mechanisms of pH-responsive nitrogen-containing MOFs as oral drug carriers were further explored through rat pharmacokinetic experiments, the everted gut sac experiments, and intestinal absorption mechanism experiments. The experimental results show that there is a strong electrostatic interaction between anionic drug LOX and UiO-66-PDC under simulated gastric acid environment, which prolongs the half-life of the drug, proving that LOX@UiO-66-PDC is a promising new oral drug delivery system.
研究领域:
材料科学
·
药学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）