JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Chunfeng Mao,Kai Yin,Chenghan Yang,Guomeng Dong,Guokai Tian,Yiwei Zhang,Yuming Zhou
Controlling the spatial confinement effect and highly dispersed Pd nanoparticles (NPs) can help to improve applicability in catalysis, energy conversion, and separation. However, the nonspatial confinement effect, agglomeration of Pd NPs of catalyst and harsh reaction conditions have become the urgent problems to be solved in Suzuki-Miyaura cross-coupling reaction. Herein, we report the first application of a new MOFs@COFs by using core with metal organic frameworks (MOFs) NH 2 -MIL-101(Fe) and shell with covalent organic frameworks (COFs) for loading Pd NPs. The quickly formation of a transition state, the highly dispersed Pd NPs and the advancedly spatial confinement effect were achieved by coupling Fe base synergistic active components, electron-oriented anchoring with controlling pore scale, respectively. Most notably, as a proof-of-concept application, the high catalytic activity of NH 2 -MIL-101(Fe)@Pd@COFs( 3 + 3 ) in catalysis is elucidated for Suzuki-Miyaura coupling reaction by the broad scope of the reactants and the preeminent yields of the products, together with excellent stability and recoverability. With this strategy, the mechanism of Suzuki-Miyaura coupling reaction was verified by examining the catalytic activity. We hope that our approach can further facilitate the study of the design and use of functional MOFs@Pd@COFs materials.
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Small
·
2019
·Vol. 15
·期 17
·1805478
·
IF 10.856
Kai Jia,Jiahua Ye,Guoxin Zhuang,Zanyong Zhuang,Yan Yu
Fabrication of low-dimensional nano-MOFs as well as nanoparticles/metal-organic frameworks (MOFs) hybrids has sparked new scientific interests but remains a challenging task. Taking Cu 3 (BTC) 2 as a proof of concept, it is demonstrated thats NH 3 ⋅H 2 O solution of a confined pH value can readily shape the bulk Cu 3 (BTC) 2 into nanoscale Cu 3 (BTC) 2 , beyond the need to control the crystal growth kinetics of MOFs. Adjusting the pH of NH 3 ⋅H 2 O within a much small range (10–11) allows fine tuning over the size and shape of nanoscale Cu 3 (BTC) 2 . Particularly at pH = 11, NH 3 ⋅H 2 O exhibits weak reducibility that triggers a reduction of part of Cu 3 (BTC) 2 into Cu 2 O, while shaping the other into Cu 3 (BTC) 2 nanowires. Benefiting from the coincidence of reduction and etching effects, the newly generated Cu 2 O dots can in situ anchor onto adjacent Cu 3 (BTC) 2 nanowires at highly dispersive state, forming a well-defined sponge-like architecture built of Cu 2 O dots and nano-Cu 3 (BTC) 2 . The CuO x derived from annealing of the Cu 2 O dots/nano-Cu 3 (BTC) 2 hybrid preserves the sophisticated sponge architecture and high porosity, and exhibits promising applications in phenol scavenging, with efficiency outperforming its counterparts and many other Cu-based catalysts reported in literature. It is anticipated that the findings here pave the way for the rational design of intricate nano-MOFs in a more efficient way.
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CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Ying Zhang,Jiabin Zhou,Xin Chen,Luo Wang,Weiquan Cai
In this work, a Fe-based metal organic frameworks (MIL-88A) has been synthesized through a hydrothermal method and adopted as a high-efficiency catalyst for photocatalysis (PC) coupled with sulfate radical-based advanced oxidation processes (SR-AOPs) to degrade tetracycline hydrochloride (TC-HCl) under visible light irradiation. The effects of MIL-88A/persulfate (PS) molar ratio, initial solution pH and catalyst dosage were studied. The results indicated that the combining of the photocatalysis and SR-AOPs could remarkably enhance TC degradation and 200 mg/L 100 mL TC could be degraded completely at 0.25 g/L MIL-88A, unadjusted pH value and 4 mM PS in 80 mins. The results of scavenging experiments and ESR analysis demonstrated that SO 4 − • and •O 2– radicals were the predominant radicals for the TC degradation. The significant improvement of degradation rate in MIL-88A/PS/Vis process is attributed to the following two factors: (1) as a photocatalyst, MIL-88A could be excited by visible light, therefore photogenerated electrons (e − ) on the conduction band (CB) of MIL-88A could be trapped by PS to generate SO 4 − • radicals. In this process, PS acted as an electron acceptor and the electron/hole recombination was suppressed leading to the enhanced photocatalyst efficiency; (2) The PS can be activated not only by photoelectrons but also Fe (III) in MIL-88A leads to the generation of SO 4 − • radicals more rapidly and easily. A possible mechanism and degradation pathway for TC was proposed based on the trapping/ESR experiments and liquid chromatography-mass spectrometry (LC-MS) analysis. This work proposed a new idea and method in combining two oxidation processes in degradation of organic pollutants thus could be potentially used in environmental purification.
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CRYSTENGCOMM
·
2019
·Vol. 22
·期 5
·878-887
·
IF 3.382
Ce Wang,Zheng Yin,Zhao Cheng,Wei-Min Ma,Xi-Yao Li,Xiao-Ting Hu,Rong Shi,Ao-Wei Chen,Yang-Min Ma
Ionic MOFs are rare but function in an interesting manner due to charged frameworks and the existence of counter ions in the channels. Using one of the most simple and cheap ligands of benzene-1,3,5-tricarboxylic acid (H3btc), we constructed five novel anionic MOFs namely [Me2NH2][Cd(btc)]·0.5DMA·2H2O (1), [Me2NH2]2[Cd5(btc)2(lac)3(H2O)3]·4DMF (2, H2lac = 2-hydroxypropanoic acid), [Me2NH2][MnII(btc)]·DMA (3), [Me4N]3[MnII3(btc)2(Hbtc)(CH3COO)]·9CH3OH (4) and [Me2NH2]2[Zn5(btc)4(DMA)2]·5.5DMA (5). Rich structure variabilities including cluster-based, pillared-layer and rod-spacer motifs were found in these MOFs because of the different metal coordination and effect of auxiliary ligands. 1 was a [Cd2(COO)4]-based porous framework belonging to (3,6) connected α-PbO2 net. 2 was a [Cd(btc)]-layers and [Cd2(lac)2] pillar-based framework, which possessed rare-ordered defects due to the self-absence of 25% pillars. In 2, for the first time, extremely rare square-planar Cd(II) geometry in porous MOFs was found. 3 was the first 3D framework constructed from unusual Mn–carboxyl chains with [Mn2(COO)2] building blocks. 4 provided a new example to construct a pillared-layer framework from self-assembled metal–ligand chains as pillars. 5 had a [Zn2]-cluster-based framework with dual pore systems of 1D rounded channels and elongated cages. A new single-phase white-emitting phosphor of 1 was found, which exhibited near-sunlight and human vision friendly broadband spectrum, with extremely large full width at half maximum (FWHM) of up to 268 nm, close pure white chromaticity coordinates of (0.303–0.317, 0.354–0.364), near daylight color temperature of 5773–5899 K, as well as high color rendering index of 90. In comparison, 2, 3 and 4 showed single and narrow blue emission. Rapid and selective capture of methylene blue (MB) over methyl orange (MO) was realized in 1, while MB adsorption in other MOFs was negligible.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Yuanming Tan,Zhongqiao Sun,Hao Meng,Yide Han,Junbiao Wu,Junli Xu,Yan Xu,Xia Zhang
MOFs/polymer hybrid membranes combine the special surface activity of MOFs and the excellent carries nature of porous polymer and thus exhibit unexpected adsorption/separation performances in the solid-phase extraction. In this paper, a new kind of MOFs/polymer composite membrane , MIL-68(Al)/PVDF have been fabricated for the first time through blending the MIL-68(Al) nanoparticles and polyvinylidene fluoride (PVDF) casting solution and following the lyotropic phase transition. Some means such as SEM, XRD and FT-IR are used to character the structure of these hybrid membranes. The membrane performances including the hydrophilic/hydrophobic properties, membrane porosity and membrane water flux are also measured. The effects of doping amount of MIL-68(Al) on the structure and performances of MIL-68(Al)/PVDF hybrid membranes are discussed. Two persistent organic pollutants : p -nitrophenol (PNP) and methylene blue (MB) are chosen as main adsorption objects to evaluate the adsorption activity of MIL-68(Al)/PVDF hybrid membranes. The influences of various conditions on the adsorption activities are investigated in detail and the optimum adsorption conditions are determined. All the MIL-68(Al)/PVDF hybrid membranes exhibit enhanced adsorption capacity compared to pristine PVDF, and the adsorption activities of hybrid membranes are promoted continually with the increasing doping contents of MIL-68(Al). The adsorption thermodynamics analysis indicates that the adsorption process is mainly characterized by Langmuir monolayer adsorption and chemical adsorption . The coordination bonding formed between NO 2 of PNP and Al(III) of MIL-68(Al), and the acid-base interaction between the sulfur of MB and Al(III) of MIL-68(Al) may be responsible to the highest removal efficiency of PNP and MB. The good dynamics adsorption and regeneration performances indicate the prospect applications of these MOFs/PVDF hybrid membranes in the separation of organic contaminants from industrial waste water.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Tiantian Li,Zhining Huang,Mengfan Hu,Yuen Hu,Ke Quan,Man Zhou,Yao chen,Shaoju Fu
Heavy metal wastewater pollution has been a globally important and serious issue for the industrial manufacturing center. Herein, we developed a novel CAP@Ui0-66-NH 2 @PPy nanocomposite fibrous membrane, by combining the in-situ growth and oxidative polymerization technical routes, which possessed a high specific surface area and abundant amino-active sites to remove Cr (Ⅵ). Systematic characterization showed that the porous structure and in situ growth of MOF provided sites for polymerization of charged polypyrrole (PPy), resulting in the large specific surface area (78.837 m 2 /g) of CAP2@Ui0-66-NH 2 @10 %PPy. The maximum adsorption capacity was as high as 312.70 mg/g at 298 K, which was significantly better than that of CAP (CA and PVP electrostatic spinning and then washing off the PVP) nanomembranes. The adsorption process was consistent with the proposed secondary kinetic and Langmuir model, and the high adsorption capacity was maintained after five rounds of cyclic adsorptions. Through XPS analysis, the abundant amino groups on the surface of the adsorbent material were protonated, caused the electrostatic attraction and ion-exchange interaction with the anion Cr(Ⅵ). These protonated amino groups were able to reduce the toxic Cr (Ⅵ) to non-toxic Cr (Ⅲ), which was immobilized on the surface of the material through chelation. The MOF lattice achieved in-situ growth on porous CA nanofibrous membranes, which significantly enhances the mass-transfer dynamics and the membrane cycling stability, the amine-based functionalization of the UI0-66-NH 2 improved the coordination activity and increased the adsorption efficiency, and polypyrrole (PPy) conductive layer promoted the directional migration of Cr (VI) and effectively suppressed the interference of competing ions. In sum, the prepared CAP@Ui0-66-NH 2 @PPy hybrid fibrous membranes showing great potentially applicable for heavy-metal wastewater treatment.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2025
·
IF 2.8
Junying Wu,Ruijie Guo,Houting Kang,Yanming Wang,Jingyuan Tian,Jierong Wang,Hong Yan
Metal–organic frameworks (MOFs) have great potential in improving the fire safety of polymer materials. To improve the fire resistance and smoke suppression of polypropylene (PP), a flame-retardant system ZIF-67@γ-CD-MOFs@APP incorporating multiple flame-retardant elements was designed and applied to PP. The coated PP passed UL-94 V-0 level with the LOI up to 36.2% and char residue of 12.47%. The PHRR, PSPR, COP, and CO 2 P of coated PP were reduced by 52.65%, 24.72%, 36.49%, and 52.29%, respectively, compared to neat PP. In addition, the tPHRR, tPSPR, tCOP, and tCO 2 P were prolonged by 405.3%, 345.4%, 427.8%, and 405.3% compared to pure PP, allowing more escape time when facing a real fire. Integrating the hierarchical porous structure provided by ZIF-67 and γ-CD-MOFs, catalytic carbonization of transition metal Co and the nitrogen-containing ligand, ZIF-67@γ-CD-MOFs@APP played a flame-retardant role both in the condensed and gas phase, endowing PP with enhanced flame retardancy and smoke suppression. The “all-in-one” strategy provides helpful insights for constructing fire retardant system with multi-level nanostructure.
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SPECTROSCOPY LETTERS
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2025
·
IF 1.6
Shuaibin Wu
In this study, a novel surface enhanced Raman scattering (SERS) substrate material was designed and prepared for the real-time Rhodamine 6 G SERS detection. Firstly, ZIF-67 was modified on the surface of polypropylene membrane by in-situ growth methods. Subsequently, the pre-prepared Ag nanoparticles were modified on the surface of the polypropylene membrane through the covalent reaction. The result of scanning electron microscopy characterization showed that Ag nanoparticles was modified on the surface of ZIF-67 through simple electrostatic adsorption and the chemical reaction of the Ag-S bond; The infrared characteristic peaks of ZIF-67, as well as the x-ray diffractometer and x-ray photoelectron spectrometer characteristic peaks of ZIF-67 and Ag nanoparticles could all be identified. On the other hand, based on this material, we have investigated the feasibility of conducting real-time SERS detection under optimized conditions when the sample was in a flowing situation. The experimental results showed that the SERS detection of Rhodamine 6 G could be completed within 15 min in the mode of real-time, with an relative standard deviation of 10.67%. The concentration of Rhodamine 6 G and the intensity of the SERS signal also have a good linear relationship within the range of 103, 5 × 102, 2.5 × 102, 25 and 10 μmol/L.
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Sustainability
·
2024
·Vol. 16
·期 5
·1945
·
IF 3.3
Zhongming Wu,Jianxin Deng,Tuanwei Zhao,Yang Zhou,Yongfu Kang,Xiangxiang Bai,Fei Hong,Longfei Fu,Gensheng Li,Zhiyi Zhang,Weiming Guan
Rapid economic development and increased demand for mineral products in China have led to extensive extraction of various ores, resulting in significant environmental challenges associated with the generation of industrial solid waste, particularly iron tailings. Despite being a major mining nation, China faces issues of wasteful practices, with substantial amounts of valuable elements lost during the processing of iron ore. This study addresses the urgent need for sustainable solutions by proposing an innovative approach for the recovery of valuable elements from iron tailings. The proposed process involves a sequential application of acid leaching, chemical precipitation, and Metal-Organic Frameworks (MOFs) ion adsorption. The pre-treated iron tailings were leached in HCl solution with pH 1.5 at 70 °C for 2 h, and the co-leaching efficiency of 98.1% V, 98.2% Mo, 99.3% Fe, and 98.7% Mg was obtained. Chemical precipitation is then employed to isolate Fe, Mg V, and Mo and promote the formation of targeted compounds, ensuring concentration and purity. The integration of MOF ion adsorption, known for its high surface area and tunable pore structures, provides an efficient platform for selectively capturing and recovering target ions. 97.7% V and 96.3% Mo were selectively extracted from Zirconium 1,4-carboxybenzene metal-organic framework (UiO-66) adsorption system with pH 5.0 at 30 °C for 6 h, and 91.7% V and 90.3% Mo were selectively extracted from 2-methylimidazole zinc salt metal-organic framework (ZIF-8) adsorption system with pH 5 at 30 °C for 6.0 h. This three-stage process offers an efficient method for the recovery of valuable elements from iron tailings.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yu Liu,Mingyang Xu,Lingxin Zhao,Shufei He,Likui Feng,Liangliang Wei
The dissemination of antimicrobial resistance (AMR) in wastewater treatment poses a severe threat to the global ecological environment. This study explored the effectiveness of photocatalysis in inactivating antibiotic resistant bacteria (ARB) and quantitatively clarified the inhibiting rate of the transfer of antibiotics resistance genes (ARGs). Herein, the magnetic heterojunction as UiO-66-NH 2 @CuFe LDH-Fe 3 O 4 (UN-66@LDH-Fe) effectively facilitated the electron-hole separation and accelerated the photogenerated charge transfer, thereby guaranteeing the stable practical application in aeration tanks. Notably, the internal electric field of heterogeneous photocatalyst resulted in significant increase of ARGs inactivation, achieving 5.63 log of ARB, 3.66 log of tet A and 3.57 log of Ampr genes were photodegraded under optimal reaction conditions within 6 h. Based on the complex microbial and molecular mechanism of multiple-ARB communities inactivation in photo-treatment, the photogenerated reactive oxygen species (ROSs, ·OH and ·O 2 − ) effectively destroyed bacterial membrane protein, thereby the intracellular ROSs and redox cycles further induced oxidative stress, attributing to the abundance reduction of ARGs and their host bacteria. Moreover, long-term (7 days) continuous operation preliminarily verified the practical potential in reducing AMR spread and developing wastewater treatment efficacy. Overall, this study presented an advantageous synergistic strategy for mitigating the AMR-associated environmental risk in wastewater treatment.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2025
·
IF 4.7
Yinming Fan,Yuanzhen Li,Siqi Jiang,Yanping Zhang,Yinian Zhu,Shengpeng Mo,Lei Liao,Yanan Zhang,Xiaobin Zhou,Zongqiang Zhu
Volatile organic pollutants (VOCs) can serve as an alternative to ammonia for NO reduction, thereby enabling the simultaneous removal of VOCs and NO. In this study, different morphologies of MnO x /CoO x catalysts derived from MOFs were controllably synthesized under various hydrothermal synthesis conditions for the simultaneous removal of 1,2-propanediol and NO. Among the various samples, sample A, characterized by its rod-like structure, demonstrated superior catalytic activity. It achieved simultaneous photothermal coupling for the degradation of 1,2-propanediol and NO under UV irradiation at 240 °C, with conversion rates reaching 52 % and 67 %, respectively. The morphology of the catalysts significantly influences their catalytic performance. The incorporation of Mn increased the structural disorder of the material, thereby reducing the coordination order of Co. This significant change in the coordination environment modulates the intrinsic catalytic activity of the samples, leading to distinct catalytic properties. Furthermore, the catalytic reaction mechanisms were clarified utilizing in-situ DRIFTS combined with calculations based on Density Functional Theory. Sample A, featuring abundant unsaturated cobalt and manganese defects within its distinctive coordination configuration, greatly promoted the conversion of 1,2-propanediol into crucial intermediate species. This study presents a novel approach for the synergistic removal of VOCs and NO x .
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Weizuo Li,Rui Fu,Jing Shi,Zhenhao Xiao,Yue Xu,Dafang He,Guangyu He,Haiqun Chen,Mingchen Xie
Through in-depth study of the properties and reaction mechanisms of catalysts, it is possible to better optimize catalytic systems and improve reaction efficiency and selectivity. This remains one of the challenges in the field of catalysis. Therefore, the research and design of catalysts play crucial roles in understanding and optimizing catalytic reaction mechanisms. A robust 2D zinc-based MOFs (Zn-HA) supported Co(II) ion catalyst (Zn-HA@Co) has been designed and synthesized via a coordination-assisted strategy for β-alkylation of secondary alcohols with primary alcohols. The characterization demonstrated that the anchoring of Co(II) on Zn-HA via coordination could efficiently enhance the Co(II) ion dispersity and interaction between Co(II) and Zn-HA MOFs. Importantly, the density functional theory results have provided mechanistic insights into the energy of the HOMO and LUMO of the Zn-HA@Co catalyst as well as the energy change of the entire process after interacting with the reactants and the specific energy changes of each orbital. The synthesized Zn-HA@Co MOFs effectively lower the energy barrier of the catalytic reaction process. We expect that our research and design of catalysts will serve as valuable guideline for understanding and optimizing catalytic reaction mechanisms.
研究领域:
材料化学
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催化科学
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理论化学
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