SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xingyu Zhang,Lin Chen,Longjie Jiang,Liang Zhu,Chuqing Cao,Wei Zhang,Linting Zhao,Jiaqi Xu,Han Liu
In the advent of the new energy era, the global demand for lithium is increasing rapidly. The recovery of Li + and Co 2+ from the leachate of high-quality spent lithium-ion batteries (LIBs) offers significant economic and environmental benefits. This study proposes a TFC-ON-MOF membrane prepared through a combination of in situ growth and interfacial polymerization (IP) for the recovery of Co 2+ and Li + from battery leachate. Operated in an electrodialysis (ED) system, the experimental results demonstrated that the optimum Li + membrane flux was observed to reach 1.02 μmol cm −2 min −1 at 7.5 mA cm −2 , with the selectivity remaining at 19.84, which exemplifies well-separation and permeation performance. Following several operational cycles, the separation performance remained stable, and the membrane exhibited enhanced fouling resistance relative to commercial monovalent selective cation exchange membranes (CSO). The composite membrane features sub-nanometer windows and nanometer-sized cavities, enabling selective permeation of Li + while simultaneously sequestering Co 2+ . The inclusion of auxiliary permeation groups (PSS) also enhances overall permeation performance and selectivity. The findings contribute to the design of composite metal–organic frameworks and provide a novel approach for the selective separation of heavy metal ions from spent lithium batteries, thereby promoting the efficient recycling of valuable metal resources.
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Materials
·
2024
·Vol. 17
·期 9
·2103
·
IF 3.1
Pengfei Zhu,Qiaosen Yuan,Na Li,Zhaoxia Hu,Shouwen Chen
The development of efficient catalysts with longevity to remove chlorobenzene is challenging due to Cl poisoning. Herein, a series of Mn-Cr/ZrOxcatalysts supported by Zr-based metal-organic framework (UiO-66)-derived ZrOxwas prepared and investigated for chlorobenzene (CB) catalytic oxidation. MnCr/ZrOx-M prepared via a wet impregnation method presented an amorphous structure, indicating the homogeneous dispersion of Cr and Mn, which improved acid and redox properties. 40Mn7Cr3/ZrOx-M exhibited the best catalytic activity for chlorobenzene oxidation with T90of 293 °C, which is mainly due to the strong interaction between manganese and chromium promoted by the large specific surface area of the ZrOxsupport. Furthermore, 40Mn7Cr3/ZrOx-M presented excellent stability for chlorobenzene oxidation.
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Desalination and Water Treatment
·
2024
·
IF 1
Yang Shen,Fatoye Sawyerr,Lunbo Xu,Shusu Shen,Xiaoji Zhou
The preparation of modified membranes utilizing the UiO-66 framework for wastewater filtration is regarded as one of the most promising approaches to wastewater treatment, owing to its high efficiency and cost-effectiveness. In this study, a post-modified MOF, UiO-66-RSA, was synthesized via the condensation reaction of UiO-66-NH 2 and 2,4-dihydroxybenzaldehyde. PVDF mixed matrix membranes (MMMs) were fabricated for the first time by mixing UiO-66-RSA into PVDF using the non-solvent induced phase separation (NIPS) method. Compared to pure PVDF membranes, the newly developed membrane, M4, demonstrated enhanced compatibility and superior mechanical strength. In dyeing wastewater treatment applications, M4 showed excellent separation efficiency for dye and heavy metal mixed wastewater, achieving rejection rates exceeding 90 %. Additionally, it maintained a high flux recovery rate (FRR > 90 %) and rejection rate (Rejection > 90 %) after six filtration cycles of dye-containing wastewater, indicating strong recyclability. These findings suggest that MMMs embedded with UiO-66-RSA hold significant promise for dyeing wastewater treatment.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 8
·3573-3580
·
IF 2.7
Ruidong Li,Bo Zhao,Ganggang Chang,Shanchao Ke,Minjie Chen,Didi Dong,Chun Pu,Xiaoyu Yang
In the current investigation, the base-metal hollow multifunctional catalyst, Pd–IL@H-UiO-66-NH2, was fabricated utilizing a hydrothermal method followed by etching and supporting processes. The results of the effort demonstrate that Pd–IL@H-UiO-66-NH2 displays significantly enhanced activity and product selectivity in catalysis of the one-pot Knoevenagel condensation–hydrogenation reaction, as well as a high level of generality in promoting hydrogenation reactions of unsaturated hydrocarbons. The excellent properties of Pd–IL@H-UiO-66-NH2 are ascribed to its rationally designed spatial distribution of catalytically active sites within its hierarchical structure, which is comprised of surface wrinkles that increase hydrophobicity and exposure of the active sites, and hollow structures that serve as nanoreactors to enrich substrate interactions and improve mass transfer. Furthermore, the catalytic stability of Pd–IL@H-UiO-66-NH2 was shown to be largely maintained after its use in five successive catalytic cycles. The stability of the new tandem catalyst benefits from strong confinement effects associated with its hollow structure and electronic interactions between the Pd and ILs that effectively restrict leaching and aggregation of Pd nanoparticles (NPs).
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu
A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.
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ChemistrySelect
·
2024
·Vol. 10
·期 1
·e202405135
·
IF 1.9
Zhanmeng Liu,Mang Lu,Haitao Gan,Jiacheng Li,Guiqing Gao,Manqing Xu,Xianglian Wang
Graphical OTC molecules diffuse to the surface of FU3 to cause film diffusion, and continue to diffuse and fill into large-, medium- and micro-pores of FU3. FU3 can be π─π conjugated and cation─π bonded with the benzene rings and amino groups of OTC. The charged surface of FU3 leads to a strong electrostatic effect in the adsorption process. The doping of Fe 3 O 4 produces structural defects to promote the OTC adsorption. As one of the most stable metal-organic frame materials (MOFs), UiO-66 has attracted extensive attention in the adsorption field. However, the application of UiO-66 is still constrained by the weak electron-hole charge separation capability and the low accessibility of micropores. In this study, the mesoporous defects of UiO-66 were constructed with acetic acid and doped with Fe 3 O 4 to prepare magnetically recyclable Fe 3 O 4 @UiO-66. The doping of Fe 3 O 4 resulted in the formation of denatured mesoporous defects in UiO-66, which was conducive to adsorption oxytetracycline (OTC) in water. The crystal structure and physicochemical characteristics of Fe 3 O 4 @UiO-66 were examined. By using the static adsorption technique, the adsorption characteristics and mechanism of OTC on Fe 3 O 4 @UiO-66 were investigated. The results reveal that Fe 3 O 4 @UiO-66 has an adsorption capacity of 210 mg g −1 and an OTC removal ratio of 84.0%. The pseudo-second-order kinetics, Elovich, and Langmuir isothermal adsorption models were all applicable to the adsorption process. The adsorption process increased entropy and was an endothermic reaction. Solution pH has a little effect on the adsorption performance. This study provides the possibility of one-step synthesis of MOFs that can efficiently adsorb tetracycline antibiotics in water with low cost and excellent recyclability and reusablity.
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JOURNAL OF CHROMATOGRAPHY A
·
2025
·
IF 4
Xuejing Lou,Yingge Hao,Huina Zhou,Zhen Song,Youmei Wang,Minghua Lu
The creation of defects in crystalline structures can tune metal-organic frameworks (MOFs) properties, such as improving their adsorptive and catalytic performance with producing more porosity and active sites. In this work, the bimetallic UiO-66 containing Zn and Zr was prepared. And then UiO-66 with missing cluster defects (UiO-66-1/3) were obtained by acid washing to remove the Zn nodes. UiO-66-1/3 was used as sorbent of dispersive solid-phase extraction (dSPE) to extract and enrich (BUs). Combination with high-performance liquid chromatography-diode array detector (HPLC-DAD) was developed to detect trace BUs in soil samples. Adsorption equilibrium can be reached in 3 min. The method possesses high enrichment factor (202-325), low detection limit (0.005-0.04 ng·mL -1 ), and wide linear range (0.02-200 ng·mL -1 ). In addition, the recovery rate of UiO-66-1/3 as an adsorbent was still higher than 95% after reused for 16 times. This work provides a new material for the enrichment and detection of benzoylurea insecticides in the environment.
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LANGMUIR
·
2024
·
IF 3.7
Ding Wang,Xiaohua Jia,Zhiqiang Shan,Li Gao,Jin Yang,Zhaofeng Wang,Haojie Song
Fluorinated graphene (FG) among numerous two-dimensional materials has enormous potential in improving antifriction properties. However, they being susceptible to thermal oxidation and prone to wear hinder practical applications. Herein, UIO-66-NH2 (Zr-MOF) enjoying good chemical and thermal stabilities was assembled on the surface of FG nanosheets under covalent bonds and van der Waals forces. The Zr-MOF@FG composite was successfully synthesized and used as a lubricant additive. It can be seen that Zr-MOF@FG composites offer a synergistic lubricant mechanism at the friction interface. Moreover, due to the adsorption and purification performance of Zr-MOF, the obtained Zr-MOF@FG composite adsorbs the abrasive rust during the friction process, thereby realizing the purification of the lubricant. These findings suggest that Zr-MOF@FG shows tremendous potential as a lubricant additive.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Lu Lin,Yongjian Zeng,Suyu Zhang,Di Hu,Zhiwei Jiang,Guoqing Guan,Kai Yan
The hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) to biofuel 2,5-dimethylfuran (DMF) serves as a vital reaction in biomass refineries. Herein, Pd-UiO-66 catalysts with controlled contents of ligand-vacancies were developed for the HMF-to-DMF conversion. Strikingly, a volcano-like relationship between defect level and HDO activity was obtained. The DMF yield was promoted ∼3 times, reaching 92.2 % at 160 °C and 15 bar H 2 , which refers to a high-level turnover frequency value of 42.66 h −1 among the reported candidates. The Pd-UiO-66 catalysts also afforded >80 % yield for the HDO of 5-methyl furfural, furfural, and vanillin. Besides, high HDO activity could be retained in five recycles. Manipulating the contents of ligand-vacancies was confirmed to create more Pd 0 species and Bronsted acid sites, leading to remarkable performance. This work provides significant inspiration for tuning structural defects in MOFs to realize the efficient HDO of platform molecules in biomass valorization.
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CRYSTENGCOMM
·
2024
·
IF 2.6
Hao He,Xiao-kai Liu,Bai-yun Zhao,Li-juan Zhou,Xuan Zhao,Chen-xu Wang,Ji-yuan Zhang,Yuan-fang Zhang,Li Wang
In this study, UiO-66-NH2 nanoparticles were synthesized via a hydrothermal method, using acetic acid and hydrochloric acid as modulators to optimize the specific surface area and pore width. Oxytetracycline (OTC) was chosen as the test compound to evaluate the adsorption efficiency of UiO-66-NH2.The material was thoroughly characterized under varying conditions, and the adsorption mechanism was systematically explored through adsorption kinetics, isotherms, and thermodynamic analyses. The results demonstrated that UiO-66-NH2 exhibited a high OTC adsorption capacity, achieving a maximum of 312.5 mg g−1 under optimal conditions. XRD, TGA, and BET analyses revealed that acetic acid and hydrochloric acid significantly improved the crystallinity and thermal stability of UiO-66-NH2, increasing the specific surface area from 8.023 m2 g−1 to 998.663 m2 g−1 and reducing the pore width from 18.783 nm to 2.129 nm. FTIR, XPS, adsorption kinetics, and isotherm studies indicated that the main forces driving OTC adsorption by CMC-Fe were hydrogen bonding, π–π stacking, weak electrostatic interactions, and pore filling. Cyclic adsorption experiments further demonstrated the excellent reusability of UiO-66-NH2. In summary, the use of acetic acid and hydrochloric acid significantly increased the specific surface area of UiO-66-NH2, exposing more adsorption sites and playing a critical role in pollutant removal.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xun Liu,Yufei Shu,Mengxia Wang,Weiwen Chen,Aling Wan,Zhongying Wang
Efficient and selective removal of fluoride from water remains a critical challenge in environmental remediation. In this work, we report a thermally modulated strategy to enhance the electrosorption performance of cerium-based metal–organic frameworks (UiO-66(Ce)) for fluoride removal. Rather than complete carbonization, controlled partial carbonization at 400 °C was found to be optimal, inducing the in situ formation of well-dispersed CeO2 nanoparticles and the development of interconnected mesoporous channels. The evolution of the pore structure with different thermal treatment temperatures was comprehensively characterized by N2 adsorption–desorption analysis and high-resolution transmission electron microscopy (HRTEM). This approach effectively balances electrical conductivity and active site availability, leveraging a nanoconfinement effect that restricts CeO2 aggregation, preserves active sites, and facilitates efficient ion transport. The optimized UiO-66(Ce)-400 °C material exhibits a high electrosorption capacity of 73.7 mg·g–1, rapid kinetics, and strong fluoride selectivity in the presence of competing anions. Finite element simulations and electrochemical analyses confirm that the synergy between enhanced mesoporosity, conductivity, and active site accessibility drives superior performance. Furthermore, the electrode demonstrates excellent regeneration and stability over five cycles. This study presents a versatile and scalable approach for engineering MOF-derived materials, offering valuable insights into the design of next-generation electrosorption systems for water treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiangyang Liu,Jin Wang,Wenyue Huang,Maogang He
Difluoromethane (R32) is a good additive to improve the coefficient of performance (COP) of hydrofluoroolefins (HFOs) which are the next generation of refrigerants. Therefore, it is important to efficiently recover Difluoromethane (R32) from R410A(a blend of 50 % R32 and 50 % pentafluoroethane (R125)) which will be eliminated due to high global warming potential (GWP). In this work, fluorinated UiO-66 was synthesized by replacing the terephthalic acid ligand in UiO-66 with an organic ligand containing fluorocarboxylic acids to enchance the separation performance of mixed matrix membranes (MMMs) as filler, and the effect of the fluorine content of the fluorinated UiO-66 was investigated. In this study, Fluorinated UiO-66/Pebax MMMs were successfully prepared, with the fluorine content tailored by using different ligands. The separation performance increased with the amount of fluorine in the MOFs, namely UiO-66-(CF 3 ) 2 /Pebax > UiO-66-F 4 /Pebax > UiO-66-F 2 /Pebax > UiO-66-F/Pebax > UiO-66/Pebax MMMs. The 20 wt% UiO-66-(CF 3 ) 2 /Pebax achieved an ultra-high P R32 of 979.53 Barrer (397 % of pure Pebax membrane) while maintaining a high ɑ R32/R125 (16.64, 251 % of pure Pebax membrane).The tested results showed that the fluorinated UiO-66/Pebax MMMs sigificantly improved permeability and selectivity for R410A due to the higher R32 solubility caused by C-F…H hydrogen bonding network formed between the fluorine groups and R32 as well as the better sieving ability caused by the decrease in the pore size of UiO-66. The fluorinated MOFs/Pebax MMMs prepared in this work simultaneously achieved better R32/R125 selectivity and R32 permeability,than the exsited membranes, enabling effective separation and recycle R32 from R410A.
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