INORGANIC CHEMISTRY
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2025
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IF 4.7
Chao Yang,Hao Chen,Yuankai Li,Zhelin Su,Yeshuang Wang,Xufei Liu,Huiling Fan
The low sulfur selectivity of Fe-based H2S-selective catalytic oxidation catalysts is still a problem, especially at a high O2 content. This is alleviated here through anchoring FeOx nanoclusters on UiO-66 via the formation of Fe–O–Zr bonds. The introduced FeOx species exist in the form of FeIII and FeII. Therein the FeIII–O species are the predominant active sites for H2S-oxidation. The formed Fe–O–Zr bonds strengthen the redox cycle of FeIII/FeII through promoting electron transfer from Fe to Zr. The FeII–O species can activate molecular oxygen to oxidize H2S into elemental S, which accelerates the formation rate of atomic S, hindering its further oxidation into SO2. The combination of these factors empowers the catalysts, enabling 100% H2S conversion and 98.2% sulfur yield. The catalyst also has satisfactory stability with the sulfur selectivity only decreasing from 98.2% to 91.3% after the reaction going on 50 h. The decreased sulfur selectivity might be caused by the deterioration of pores and the deposition of elemental S on the surface. The former hinders the diffusion of sulfur oligomers timely from pores to the gas phase, while the latter is suspected to capture electrons to promote its further reaction with molecular oxygen.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Liwei Qian,Yuhao Zhang,Wenqi Song,Sufeng Zhang,Nan Zhang,Valentin Nica
Glycoproteins are essential in biological systems, yet their complex structures and diverse glycosylation patterns present challenges for efficient and specific recognition. Herein, molecularly imprinted polymers (MIPs) with high selectivity and adsorption capacity for glycoproteins were developed using two synergistic strategies. One strategy was to synthesize a boronic acid-containing ionic liquid (PBA-IL) functional monomer that combines long-range non-covalent interactions with short-range covalent bonds, enhancing the interaction modes with ovalbumin (OVA) to improve imprinting efficiency. The other strategy entailed constructing a composite carrier with high specific surface area (50.3 m 2 /g) and abundant active sites by in-situ growth of UiO-66 metal–organic framework crystals on a wood-derived cellulose sponge (WCS). This composite (WCS@UiO-66) was utilized in a template immobilization method combined with surface imprinting technique (TIM-SIT) to prepare the MIPs (WCS@UiO-66@MIPs). Molecular simulations indicated that PBA-IL formed stronger interactions with OVA compared to traditional monomer. Based on these characteristics, the WCS@UiO-66@MIPs achieved rapid adsorption equilibrium within 40 min, exhibiting surprisingly high adsorption capacity (up to 571 mg g −1 ) and recognition ability (imprinting factor of 5.09) for OVA. The competitive adsorption experiments also demonstrated the efficient extraction of OVA from biological samples by WCS@UiO-66@MIPs, confirming its exceptional specificity. Additionally, the osmotic separation experiments revealed that WCS@UiO-66@MIPs achieved a selective permeation factor of up to 7.68 for OVA in a binary protein mixture, further demonstrating their potential for large-scale continuous separation processes. Therefore, this work provides a promising strategy for the efficient and specific recognition of glycoproteins, advancing their application in biotechnology and analytical chemistry.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2013
·Vol. 19
·期 42
·14279-14285
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IF 5.831
Dengrong Sun,Yanghe Fu,Wenjun Liu,Lin Ye,Dengke Wang,Lin Yang,Xianzhi Fu,Zhaohui Li
Graphical Higher CO 2 photoreduction activity than previously studied metal–organic framework (MOF) NH 2 -MIL-125(Ti) in the presence of triethanolamine (TEOA) as the sacrificial agent under visible light is exhibited by the amino-functionalized MOF NH 2 -Uio-66(Zr). The photoinduced electron transfer from 2-aminoterephthalate linkers to Zr oxo clusters was revealed for the first time by photoluminescence studies, and the generated Zr III was detected by ESR analysis (see figure). Metal–organic framework (MOF) NH 2 -Uio-66(Zr) exhibits photocatalytic activity for CO 2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH 2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr III and its involvement in photocatalytic CO 2 reduction was confirmed by ESR analysis. Moreover, NH 2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO 2 reduction due to its enhanced light adsorption and increased adsorption of CO 2 . This study provides a better understanding of photocatalytic CO 2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO 2 reduction.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Zhiwei Wang,Guangyuan Hu,Changqing Xia,Xinliang Wang,Hongxing He,Zhifeng Nie,Shixing Wang,Weili Li
The recovery and utilization of precious metals from secondary resources are important owing to their pivotal role in modern technology. In this study, we successfully grafted diamine onto UiO-67, modulated its charge and functionalization, and developed a highly efficient adsorbent for the extraction of Au(III) from waste solutions. The recovery rate of UiO-67-(NH 2 ) 2 for trace gold is >99 % in the wide range of pH 3 to 9. The maximum adsorption capacity of UiO-67-(NH 2 ) 2 at a temperature of 298 K is 482 mg/L. In addition, UiO-67-(NH 2 ) 2 exhibits excellent selectivity to Au(III) in mixed metal ion waste solutions. After five cycles of adsorption–desorption experiments, the adsorption efficiency remains above 95 %. The identification of electrostatic interactions, coordination, and reduction as the primary adsorption mechanisms is supported by X-ray photoelectron spectroscopy (XPS) analysis of UiO-67-(NH 2 ) 2 and density functional theory (DFT) calculations.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 35
·23940-23947
·
IF 10.7
Kai Chen,Qingqing Liu,Zhiying Qiu,Huan Zhang,Ning Gong,Lihua Zhu
Pt-PMo@UiO-66 catalysts synthesized via a solvothermal method utilizing phosphomolybdic acid as a stabilizing agent exhibit exceptional catalytic performance in the selective hydrogenation of nitroarenes. The nanostructure of the Pt-PMo@UiO-66 catalysts is demonstrated by ICP-OES, XRD, XPS, TEM, HRTEM, STEM-EDS and other characterization studies. The Pt nanoparticles (NPs) or clusters are mainly supported on the surface of UiO-66. There is a synergistic catalytic effect between Pt, phosphomolybdic acid and UiO-66, improving their catalytic hydrogenation performance (activity, selectivity and stability) for nitroarene hydrogenation. It is found that 0.32%Pt-PMo@UiO-66 has the best catalytic properties for nitroacetophenone hydrogenation, with 98.8% conversion and 99.6% selectivity to aminoacetophenone under relatively mild reaction conditions (1.75 h, 40 °C, 3.0 MPa H2). The turnover frequency (TOF) reaches 1498.0 h−1. The catalyst also shows high selectivity for the hydrogenation of halogen-containing nitroarenes without dehalogenation. The appropriate size of the Pt NPs (4.44 nm) and the electronic effect (electron transfer from Pt to Mo) improves the catalytic hydrogenation activity and selectivity of Pt-PMo@UiO-66 for the selective hydrogenation of nitroarenes under moderate reaction conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yu Yang,Meng Du,Jiaxin Liang,Qian Xu,Wei Liu,Ang Li
The flow-through electroactive membrane adsorption method has been proved to be a promising strategy to enrich low-concentration phosphate. However, the challenges of selective adsorption of phosphate and poor regeneration restrict its industrial application. Here, this study proposed a novel bimetallic Mg-UiO-66@rGO electrode material through the introduction of Mg(II) into UiO-66, which possessed remarkable adsorption selectivity and optimal reproducibility among the reported electrode materials. The maximum phosphate adsorption capacity of Mg-UiO-66(13)@rGO (Zr/Mg = 3:1) was 62.81 mg⋅g −1 at 3.2 V. Furthermore, it maintained the excellent adsorption properties in the presence of all competitive anions and after 30 times of continuous adsorption–desorption. In actual wastewater, Mg-UiO-66(13)@rGO still represented excellent adsorption kinetics of 0.51 mg⋅(g⋅min) −1 and equilibrium adsorption capacity of 61.2 mg⋅g −1 . The superior selectivity of Mg-UiO-66@rGO was attributed to the establishment of coordinative unsaturated metal sites (CUMSs), thus increasing the adsorption sites. The synergic effect of electric field facilitates the breaking and formation of coordination bonds between charged ions and deeper binding sites, boosting the adsorption–desorption ability. Notably, the structural stability is also a key factor in promoting repeated material regeneration. This study advances electrode material to a new level by introducing CUMSs and bimetallic synergies.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xiao-hu Ma,Si-yuan He,Zhe-rui Zhang,Zhe Meng
Persistent light-emitting materials (PLMs), which have the potential to store and release light energy after light irradiation, are receiving increasing attention for their role in prolonging the lifetime of photogenerated electrons for the development of photocatalysts with round-the-clock applications. In this paper, a double S-scheme Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ /ZnIn 2 S 4 /UiO-66-NH 2 (SZU) heterojunction with round-the-clock catalytic activity was prepared by hydrothermal self-assembly method. The photocatalytic performance of the SZU heterojunction for RhB(MB) degradation was significantly improved compared with the pristine ZnIn 2 S 4 and UiO-66-NH 2 . The SZU heterojunction has excellent catalytic degradation performance for RhB (MB), and the removal rate of RhB (MB) reaches 72.2 % (81.7 %) after visible light irradiation for 40 (60) minutes. After the end of light, the total removal rate of RhB (MB) reached 86.7 % (96.8 %) when the catalysis continued for several hours under dark conditions, which was 14 % and 15 % higher than that under visible light irradiation, respectively. Based on the characteristics of SMS photoluminescence, combined with a large number of photocatalytic experiments, The sustained photocatalytic activity was enhanced under both daytime and darkness conditions, not only because of the production of SZU complexes, which prolonged the visible light response of ZnIn 2 S 4 , but also because of the construction of double S-scheme heterojunctions, which facilitates the light storage capacity, charge transfer, and the separation of photo-induced charge carriers and effectively promoted the photocatalytic activity of the photocatalysts. This work contributes to a deeper understanding of the design of round-the-clock photocatalysts, and provides a useful exploration for the practical application of photocatalytic technology.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Guzheng Mao,Qiqi Kan,Zhongyuan Yue,Shengui Ju,Haoli Zhou,Wanqin Jin
Pervaporation (PV) is an energy-efficient membrane technology for separating organic mixtures. Traditional polymer membranes in the PV face limitations due to a trade-off between flux and separation factor. Mixed-matrix membranes (MMMs) fabricated using solution mixing or filler modification often suffer from interfacial defects or require additional complex preparation steps. This study introduces an in situ polymerization method that incorporates UiO-66-NH 2 into the polyamide polymerization process to fabricate UiO-66-NH 2 @polyamide (PA) MMMs for methanol and dimethyl carbonate separation, which effectively resolves the interfacial defect issues while eliminating additional filler modification steps. The trade-off issue is also overcome. Results show that in situ polymerization improves UiO-66-NH 2 dispersion in the polymer matrix and strengthens polymer–filler interactions. MMMs with 5 wt% UiO-66-NH 2 loading achieved a total flux of 11.5 kg/(m 2 ·h) and a separation factor of 12.5 at 30 °C, representing a 2.32-fold and 1.46-fold improvement over pure PA membranes. These findings demonstrate the significant benefits of in situ polymerization in enhancing MMM performance and simplifying fabrication, providing an efficient strategy for industrial PV applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Ruirui Li,Wei Zhuang,Yan Gao,Yahan Bai,Keke Zhang,Zhenfu Wang
Herein, UiO-66 was selected as the immobilization carrier of Rhizomucor miehei lipase (RML). After etching and hydrophobic modification, the functionalized UIO-66 (H-UIO-66-OPA) was utilized for RML immobilization and the obtained RML@H-UIO-66-OPA showed about 70 % relative activity after incubation at 60 °C, which was much better than RML (20 %). RML@H-UIO-66-OPA was used in the synthesis of 1,3-dioleic acid glycerol (1,3-DAG) and the effects of reaction conditions (temperature, enzyme addition, substrate molar ratio, and time) on 1,3-DAG yield were investigated. Under the optimal conditions (temperature of 65 °C, enzyme addition of 2 wt%, substrate molar ratio of 2:1, and reaction time of 4 h), 1,3-DAG yield reached 77 %. Finally, Box-Behnken experimental design method was utilized to optimize the process parameters for the preparation of 1,3-DAG, and the final 1,3-DAG content was 79.80 %, which demonstrated that the model could predict the relationship between the factors and be suitable for the process optimization in 1,3-DAG preparation.
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JOURNAL OF CHROMATOGRAPHY A
·
2015
·
IF 4.169
Wenmin Zhang,Zhiming Yan,Jia Gao,Ping Tong,Wei Liu,Lan Zhang
Fe 3 O 4 @SiO 2 @UiO-66 core–shell magnetic microspheres were synthesized and characterized by transmission electron microscopy, scanning electron microscopy, X-ray diffraction, Fourier transform infrared spectrometry, vibrating sample magnetometry, nitrogen adsorption porosimetry and zeta potential analyzer. The synthesized Fe 3 O 4 @SiO 2 @UiO-66 microspheres were first used for magnetic solid-phase extraction (MSPE) of domoic acid (DA) in shellfish samples. Combined with high performance liquid chromatography–tandem mass spectrometry (HPLC–MS/MS), a fast, simple and sensitive method for the determination of DA was established successfully. Under the optimized conditions, the developed method showed short analysis time, good linearity ( r 2 = 0.9990), low limit of detection (1.45 pg mL −1 ; S/N = 3:1), low limit of quantification (4.82 pg mL −1 ; S/N = 10:1), and good extraction repeatability (RSD ≤ 5.0%; n = 5). Real shellfish samples were processed using the developed method, and trace level of DA was detected. The results demonstrate that Fe 3 O 4 @SiO 2 @UiO-66 core–shell magnetic microspheres are the promising sorbents for rapid and efficient extraction of polar analytes from complex biological samples.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Dong Wang,Tinglue Zhang,Mohamed Gamal El-Din,Xuefen Wang
In this work, the 2-fluoroterephthalic acid with asymmetric structure and high electronegative F species was introduced in the assembly of Ce-UiO-66 catalysts to increase the defect density and enlarge pore structure for enhancement in removal efficiency of sulfamethoxazole. Owing to the strong coordination ability from high electronegative F species of 2-fluoroterephthalic acid with Ce-oxo nodes, the designed CUF exhibited improved interfacial properties (accelerated electron transfer rate, available active sites and enhanced interaction with PMS), which was favorable for the exploration and accessibility of active sites with sulfamethoxazole and PMS to decrease the adsorption barrier and accelerate PMS activation. As a result, the CUF catalysts exhibited higher adsorption capacity (173.4 mg/g) than that of CUH (117.8 mg/g), the enhanced degradation efficiency of sulfamethoxazole with a rate constant higher than 2.3 times CUH, good elimination (>95 %) of methylene blue, tetracycline and ibuprofen. In addition, the CUF/PMS system possessed satisfactory stability in wide solution pH, recycling and real water and good potential application in continuous wastewater treatment based on the designed dynamic catalytic reactor. This work provided deep insight into the design of catalysts with high adsorption performance and degradation efficiency based on the structure–activity relationship.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiajun Yu,Xiao Wang,Shijie Yang,Xiaofeng Xie,Jing Sun
Ligand functionalization could effectively modulate the local electron distribution of MOFs, thus improving their performance in both the capturing and photocatalytic oxidization of various VOCs. In this work, a series of Fc-CHO/NU-X (X = 1, 2, 3, 4) were obtained through the ligand functionalization of reo -NH 2 -UiO-66 (denoted as NU) with ferrocenecarboxaldehyde (Fc-CHO) as the modifier. By altering the local charge distribution and inducing Fe-OH and cyclopentadienyl rings as new adsorption sites, Fc-CHO altered the adsorption behavior of both aromatic and oxygenated VOCs and consequently their degradation pathways. The introduction of electron-donating Fc-CHO enhanced the ligand to metal charge transfer (LMCT), accelerated the electron-hole separation and therefore promoted the effective formation of oxidative radicals, facilitating the effective oxidation of acetaldehyde. Direct charge transfer through p-p interaction enabled the ring-opening and deep oxidation of toluene. The degradation efficiencies of toluene and acetaldehyde increased from 25 % and 28 % (NU) to 80 % (Fc-CHO/NU-3) and 65 % (Fc-CHO/NU-2), respectively. Positive effects of Fc-CHO functionalization were also observed during the removal of acetaldehyde-toluene mixtures and the synergistic effect between acetaldehyde and toluene was revealed. This work provides new ideas and novel materials for the purification of in-door air pollutants.
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