JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Can Sun,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Yutong Chen,Xuewei Tu,Wenya Cai,Zhiqin Yu,Yibin Liu,Shijie Zhang,Hui Zheng
Photocatalytic nitrogen fixation is seen to be a potential technology for nitrogen reduction due to its eco-friendliness, low energy consumption, and environmental protection. In this study, photocatalysts with abundant oxygen vacancies (Zr-naphthalene dicarboxylic acid (Zr-NDC) and Zr-phthalic acid (Zr-BDC)) were designed using 1,4-naphthalene dicarboxylic acid (H 2 NDC) and 1,4-phthalic acid (H 2 BDC) as ligands. Since the structure of H 2 NDC includes one extra benzene ring than H 2 BDC, the charge density differential of the organic ligand is probably altered. The hypothesis is proved by density function theory (DFT) calculation. The abundant oxygen vacancies of the catalyst offer numerous active sites for nitrogen fixation. Concurrently, the process of ligand–metal charge transfer facilitates photo-electron transfer, creating an active center for nitrogen reduction. Additionally, the functionalization of ligand amplifies another pathway for charge transfer, broadening the light absorption range of Metal-organic framework (MOF) and increasing its capacity for nitrogen reduction. In contrast to H 2 BDC, the benzene ring added in H 2 NDC structure acts as an electron energy storage tank with a stronger electron density difference favorable for photogenerated electron-hole separation resulting in higher photocatalytic activity in Zr-NDC. The experimental results show that the nitrogen fixation efficiency of Zr-NDC is 163.7 µmol g −1 h −1 , which is significantly better than that of Zr-BDC (29.3 µmol g −1 h −1 ). This work utilizes cost-effective and non-toxic ingredients to design highly efficient photocatalysts, thereby significantly contributing to the practical implementation of green chemistry principles.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Yuqiang Liang,Hongzhi Cheng,Yujie Zhang,Junyang Jin,Yang Wang,Jian Gu,Jian Yang,Yinsheng Li
A novel amorphous Zr-MOFs (aZMs) was synthesized using ZrCl 4 and C 10 H 6 O 8 , with deionized water and ethanol as solvents. ZrC nanoparticles were successfully synthesized by pyrolyzing aZMs precursors via one-step thermal decomposition. Effects of metal/linker molar ratios and pyrolysis temperatures on the composition and microstructure of ZrC powders were investigated, meanwhile, the synthesis mechanisms were also discussed. High-purity spherical ZrC nanoparticles (104.2 ± 21.5 nm) were obtained by pyrolyzing the aZMs with metal/linker molar ratio of 2 at 1500 °C. Notably, additive-free dense ZrC ceramic were fabricated using precursor-derived ZrC nanoparticles at 1900 °C for 1 h with a pressure of 30 MPa by SPS, achieving a high relative density (96.2 %) and Vickers hardness (15.9 GPa). Compared with commercially available ZrC ceramic (93.3 %, 12.79 GPa), the as-sintered ZrC ceramic exhibited better sinterability and higher hardness. This work provides a promising potential for use in fabricating ZrC-based ultra-high temperature ceramics and composites.
研究领域:
材料科学
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陶瓷工程
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产品关联
DOI
高影响因子
Green Processing and Synthesis
·
2023
·Vol. 12
·期 1
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IF 4.3
Qinhui Ren,Yufu Ma,Fuhua Wei,Lan Qin,Hongliang Chen,Zhao Liang,Siyuan Wang
Zr-metal-organic frameworks (Zr-MOFs) were prepared by a solvothermal method and characterized by X-ray diffraction, scanning electron microscopy, and thermogravimetry. Zr-MOFs were used to remove doxycycline hydrochloride (DOC) from wastewater. According to the experimental results, the maximum adsorption capacity of DOC by Zr-MOFs within 5 h was 148.7 mg·g −1 . From the pseudo-second-order kinetics model, all R
2 values were greater than 0.99, which proved that the adsorption of DOC by Zr-MOFs was consistent with practice. According to the Freundlich isotherm model, the adsorption of DOC by Zr-MOFs proceeded via multilayer adsorption. The aforementioned results show that Zr-MOFs have good application prospects for removing DOC from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Qipeng Yang,Ru Song,Yameng Wang,Xianlong Hu,Zhiyue Chen,Zhuo Li,Weiqiang Tan
A new electrode material consisting of MOFs (Zr-TAA, TAA: trans-aconitic acid) and MWCNTs was simply synthesized by one-pot reflux method and applied to high-performance supercapacitor. With advantages of improved conductivity and uniform pore-size distribution, the composite material shows enhanced electrochemical performance with a specific capacitance of 562.06 F g −1 and retains almost 100% of its initial capacitance after 1000 cycles when measured in 6 M KOH electrolyte. Furthermore, an asymmetric supercapacitor assembled by Zr-TAA/MWCNTs-6 as positive electrode and carbon cloth as negative electrode exhibits a superior energy density of 17.53 Wh kg −1 at a power density of 902.5 W kg −1 , which demonstrates its great practical value in electrochemical energy storage applications.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang
Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Li Xia,Wenxi Zhou,Yifan Xu,Zhengqiang Xia,Xinzhi Wang,Qi Yang,Gang Xie,Sanping Chen,Shengli Gao
The introduction of rich-electron ligands is a promising strategy to improve the ligand-to-metal charge transfer (LMCT) ability of metal–organic frameworks (MOFs) for efficient photocatalytic CO 2 reduction reactions (CO 2 RR), while the resulting impaired Lewis acid sites go against stable bonding with CO 2 and hinder the electron transfering to CO 2 . It is thus the key to search a trade-off between increasing LMCT and frustrating Lewis acid. Herein, the ferrocene (Fc) modified UiO-66 series MOFs, NH 2 -UiO-66-Fc, have been prepared to optimize LMCT for boosting CO 2 RR through a simple solvent-assisted ligand incorporation (SALI) method. Theoretical calculation and systematic experiments, including photoelectrochemical measures, in situ electron paramagnetic resonance, fluorescence probe analysis and X-ray photoelectron spectroscopy indicate that with increasing Fc content, the LMCT energy of MOFs significantly decreases from 2.66 to 2.10 eV based on the established electron transfer double-channel mechanism, while the Lewis acidity of Zr sites reduces with the CO 2 adsorption energy ( E ad ) ranging from −1.061 to −0.632 eV. Through introducing an optimal Fc content, NH 2 -UiO-66-Fc (2.0) integrating satisfactory LMCT ability and Lewis acidity shows superior photocatalytic CO 2 RR performance (CO yield: 90.65 μmol·g −1 ·h −1 ), about 13 times higher than that of the unmodified MOF and superior to most reported pristine MOF photocatalysts. DFT calculation demonstrates that the excellent performance of NH 2 -UiO-66-Fc (2.0) is attributed to the lowest energy barrier of 1.50 eV for the rate-limiting step of *COOH formation. In this work, such a simple post-modification strategy for facilitating the whole electron transfer path of photocatalytic CO 2 RR will provide a new way to construct high-performance MOFs-based CO 2 RR photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2020
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IF 4.302
Jingjing Zhao,Linqiong Xu,Yaozhuo Su,Hongwei Yu,Hui Liu,Shaoping Qian,Wenge Zheng,Yongqing Zhao
ABSTRACT Zirconium-based metal-organic frameworks (Zr-MOFs) have attracted widespread attention due to their high specific surface area, high porosity, abundant metal active sites and excellent hydrothermal stability. However, Zr-MOFs materials are mostly powdery in nature and thus difficult to separate from aqueous media, which limits their application in wastewater treatment . In this study, PDA/Zr-MOFs/PU foam was constructed by growing Zr-MOFs nanoparticles on a dopamine-modified polyurethane foam substrate by in-situ hydrothermal synthesis as an adsorbent for removing dyes from wastewater. The results demonstrated that the polydopamine coating improves the dispersion of the Zr-MOFs nanoparticles on the substrate and enhances the interaction between the Zr-MOFs nanoparticles and the PU foam substrate. As a result, compared with Zr-MOFs/PU foam, the prepared PDA/Zr-MOFs/PU foam exhibits higher adsorption capacity for crystal violet (CV) (63.38 mg/g) and rhodamine B (RB) (67.73 mg/g), with maximum adsorption efficiencies of CV and RB of 98.4% (pH=11) and 93.5% (pH=7), respectively, at a concentration of 10 mg/L. The PDA/Zr-MOFs/PU foam can simultaneously remove CV and RB from the mixed solution. Moreover, the PDA/Zr-MOFs/PU foam still exhibits high stability and reusability after five cycles.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 5
·1690-1697
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IF 8.067
Mengmeng Cao,Chao Xia,Yunpeng Liu,Jinfeng Xia,Danyu Jiang,Guohong Zhou,Tongtong Xuan,Huili Li
Rapid and quantitative detection of nitrobenzene (NB) in wastewater is of great significance to protect the natural environment and human health. In this work, bifunctional Ln@Zr-MOFs based on UiO-66 were successfully fabricated by partially replacing terephthalic acid (H2BDC) ligands with m-phthalic acid (m-H2BDC) ligands and post-synthetic modification (PSM) with Ln3+ (Ln3+ = Eu3+, Tb3+). The “antenna effect” of the m-H2BDC ligands makes Ln@Zr-MOFs exhibit the characteristic emissions of Ln3+. By adjusting the amount and type of Ln3+, controllable color-tuning emissions can be easily realized, which endows them with a great application prospect for white LEDs. On the other hand, Eu10@Zr-MOFs can serve as a turn-off fluorescent switch of NB because the red emission from Eu3+ can be easily quenched by NB through a photoinduced electron transfer (PET) process between NB and its ligands, and as a result, NB is successfully recognized. Particularly, Eu10@Zr-MOFs as a fluorescent probe have shown many appealing properties, such as high sensitivity (limit of detection is 1.04 μM, limit of quantification is 3.48 μM, and Ksv = 24459.71 M−1), quick response (less than 60 s), a broad response window (0–180 μM), excellent selectivity, and strong anti-interference ability. The real detection results of NB concentration in natural water samples have demonstrated that the reported Eu10@Zr-MOFs are a potential fluorescent material that can precisely and sensitively perform fluorescence sensing of NB.
研究领域:
材料科学
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环境科学
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光学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jie Chen,Jianzhong Ma,Qianqian Fan,Wenbo Zhang,Ruyue Guo
The development of chrome-free tanning agents is of great significance for the green and sustainable improvement of the leather industry. Metal organic framework (MOFs) is a kind of nanomaterial with steady framework formed by the coordination of metal clusters with organic ligands, which gives it a natural self-masking structure. Herein, two kinds of bimetallic MOFs were obtained via post-synthesis modification and used in the tanning to produce leather with good hydrothermal stability. M n+ - replacing Zr-MOFs is denoted as Zr/M−MOFs (M n+ = Ti 4+ , Al 3+ ). Zr/M−MOFs were characterized by XRD, SEM, FT-IR, TG, XPS, and N 2 adsorption/desorption. The results indicate that M n+ - replacing provides more active site that can be combined with collagen fibers. Compared to the Zr-MOFs tanned leather (75.3 °C), the shrinkage temperature of Zr/M−MOFs tanned leather (79.9 °C) has been further improved. In addition, Zr/M−MOFs can also avoid the problems caused by traditional metal tanning, such as the worse washability of aluminum tanning. A new strategy to improve the tanning performance of MOFs-based tanning agents was provided. It gives a new approach to the development of chrome-free tanning agents.
研究领域:
材料科学
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皮革化学与工程
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环境科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Bohao Yang,Mingbo Shi,Renliang Huang,Wei Qi,Rongxin Su,Zhimin He
The treatment of oil spill and the separation of oil-water mixture have been widely concerned in recent years. In this work, a one-pot synthesis strategy is developed to prepare fluorine functionalized zirconium-based metal organic framework (Zr-MOFs) (denoted as UiO-66-1F) by using 4-fluorobenzoic acid as modulator and modifier and p-phthalic acid (PTA) as ligand. 4-fluorobenzoic acid can participate in the formation of frameworks structure and cause structural defects, causing larger surface area and hierarchically porous structure. The hydrophobicity of UiO-66-1F increases with increasing of the ratio of 4-fluorobenzoic acid to zirconium chloride and when the ratio is 10, the synthesized UiO-66-1F(10) shows high hydrophobicity with a water contact angle (WCA) of 122° while the WCA of original UiO-66 is only 21°. UiO-66-1F(10) also has good chemical stability over a wide pH range (pH 1∼11) and good hydrothermal stability. In addition, a superhydrophobic sponge (UiO-66-1F(10)@PDA@sponge) with a WCA of 150° was prepared via in situ growth of UiO-66-1F(10) on a polydopamine modified sponge (PDA@sponge). The resulting composite shows high absorption capacities for various oils and organic solvents ranging from 50.5 g/g (n-hexane)– 107.8 g/g (dichloromethane) and good recyclability.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 9
·5438-5455
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IF 4.682
Liu Boyu,Liu Moxi,Xie Zhiyuan,Li Yiru,Zhang Aibo
Metal–organic frameworks (MOFs), a new type of porous functional material, have attracted widespread attention in the field of adsorption separation, medicine, and catalysis, etc., due to their unique adjustable pore structure and large specific surface. The defective zirconium-based MOF is rich in terminal Zr–OH induced by the lack of linkers and the μ3-OH originating from the Zr cluster, exhibiting high affinity for the carboxyl and sulfonic acid groups in the dyes. We report the performance of two defective zirconium-based MOFs (MOF-808 and MIL-140C) to remove Eosin y (EY), Methyl orange (MO), and Orange g from the water. Owing to the strong affinity, larger specific surface area, and better-matched pore structure, MOF-808 exhibits higher adsorption capacity for EY and MO, with maximum adsorption capacities of 661.7 mg g −1 and 532.4 mg g −1 , respectively. The adsorption kinetics, thermodynamics, adsorption cycle performance, and adsorption mechanism of two MOFs for three dyes were investigated. Adsorption thermodynamics and XPS analysis certified that both chemical adsorption and physical adsorption occur during the adsorption process, especially chemical adsorption. Desorption and regeneration tests demonstrate that both MOF-808 and MIL-140C maintained their high adsorption capacity after four cycles, indicating two MOFs are favorable candidates for removing pollutants. Graphical abstract
In this article, the adsorption performance of MOF-808 and MIL-140C on three different sizes and structures of anionic dyes is mainly studied. The results show that MOF-808 has better adsorption performance for EY and MO. At the same time, the adsorption results show that the chemical adsorption between the adsorbate and the MOFs material plays a leading role in the adsorption, resulting in a high adsorption capacity for EY, although the EY molecule has a larger molecular size.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Fan Xiao,Xiaoyu Hu,Yingbo Chen,Yufeng Zhang
Four different thin-film nanocomposite (TFN) membranes were prepared by adding different concentrations of porous Zr-metal-organic frameworks (MOFs) (UiO-66 and UiO-66-NH2) to piperazine aqueous solution (aqueous phase) or 1,3,5-benzenetricarbonyl trichloride-n-hexane solution (organic phase) by interfacial polymerization. The main purpose is to study the specific effects of different addition methods and addition amounts of nanoparticles on the structure and performance of the TFN membranes by interfacial polymerization. All four TFN membranes exhibited a higher water permeability while maintaining high salt rejection compared to thin-film composite membrane. On the one hand, the TFN membranes behave differently, which are prepared by adding the same kind of nanoparticles to the aqueous phase or organic phase, respectively. The TFN membrane prepared by adding 0.2 w/v% UiO-66 to the organic phase had a high water flux of 87.86 L m–2 h–1, compared to 46.31 L m–2 h–1 of the membrane prepared by adding 0.3 w/v% UiO-66 in the aqueous phase. This is due to the fact that UiO-66 greatly slows the interfacial polymerization rate when UiO-66 is added to the organic phase, resulting in a thinner and wider-aperture polyamide thin-film layer, reducing the water transmission resistance during filtration. Therefore, it is more economical by adding nanoparticles to organic phase than aqueous phase under the same filtering effect. On the other hand, different nanoparticles can also cause differences in performance and structure of the TFN membranes even in the same preparation manner. TFN membrane with UiO-66-NH2 in the aqueous phase has higher water permeance than the one with UiO-66 in the aqueous phase, owing to the good hydrophilicity of the amino group, which improves the water dispersibility of UiO-66-NH2 so that the TFN membrane is more uniform. In addition, UiO-66-NH2 slows down the process of interface polymerization, making the membrane more porous. The monomers in the aqueous phase and organic phase can be adsorbed in the pores of Zr-MOFs, which makes the interfacial polymerization occur both in the pores and on the surface of the pores. Thus, the compatibility between the polyamide and MOFs was enhanced and less defects were formed in the thin-film layer, resulting in a high salt rejection even when the concentration of Zr-MOFs increased. This is the first time to explain that polyamide membrane has not obvious salt rejection attenuation with increasing porous material content using pore adsorption reaction monomer principle. Also, the Zr-MOFs-based TFN membrane exhibited good heat resistance and antifouling property. This work shows that porous Zr-MOFs nanomaterials have significant advantages in the development of nanofiltration membranes with high water flux and rejection.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）