Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Shuya Liu,Xinjie Ma,Yuxin Liu,Weiwei Chen,Yuejie Ai,Kexin Li,Xiushen Ye,Ming Fang,Xiaoli Tan
To fully utilize the customizable characteristics of metal-organic framework (MOF) materials in environmental applications, it is important to precisely modulate the branching groups of MOFs for improved performance. In this work, MIL-53(Al) was modulated by different numbers of nitrogen atoms and carboxyl groups/phosphite groups (MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 , and MOF-N 2 -(PO(OH) 2 ) 3 ) via a post-synthesis modification method, and the influence of functional groups and chain length on adsorption and the mechanism of modified groups on the adsorption of uranium (U) are demonstrated. Batch experiments suggest the removal of U(VI) reaches 37%, 27%, and 90% for MOF-N 2 -(COOH) 3 , MOF-N 3 -(COOH) 4 and MOF-N 2 -(PO(OH) 2 ) 3 , respectively (pH = 4.0, T = 25 ℃, I = 0.01 M NaNO 3 ). The surface complexation between UO 2 2+ and the surface of functional groups on the modulated MOF dominates the adsorption. Nevertheless, the steric hindrance in MOF porous structure can explain the inferiority of U(VI) adsorption on MOF-N 3 -(COOH) 4 (27%) to MOF-N 2 -(COOH) 3 (37%). MOF-N 2 -(PO(OH) 2 ) 3 is more conducive to uranyl adsorption than MOF-N 2 -(COOH) 3 or MOF-N 3 -(COOH) 4 , which is due to better affinity of U(VI) to phosphate group than the carboxyl group by density functional theory (DFT) calculation. Moreover, the excellent regeneration performance and U(VI) adsorption of MOF-N 2 -(PO(OH) 2 ) 3 in natural water or wastewater further confirmed the practical application of modulated MOFs in practical application.
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Sheng Fan,Xinru Lu,Haoliang Li,Xiaodong Du,Xiaoyu Huang,Yao Ma,Juan Wang,Xueqin Tao,Zhi Dang,Guining Lu
Organophosphate esters (OPEs) are a new class of flame retardants present in diverse waters. The study focused on the removal of aqueous OPEs using functionalized MIL-101(Fe), which was a representative of the metal-organic frameworks (MOFs). Adsorption kinetics of tris(2-chloroethyl) phosphate (TCEP), tributyl phosphate (TnBP), and triphenyl phosphate (TPhP) were investigated. Additionally, TCEP was selected as the model contaminant to study the adsorption isotherms, thermodynamics, and effect of solution matrix properties. Adsorption mechanisms obtained from the experiments were confirmed using density functional theory (DFT) calculations. Adsorption kinetics indicated that functionalized MOFs provided a significant enhancement to the removal of TCEP. The maximum adsorption capacities q m of MIL-101(Fe), MIL-101(Fe)–NH 2 , MIL-101(Fe)–OH, and MIL-101(Fe)–CH 3 at 298 K for TCEP were 76.040, 282.940, 119.680, and 181.274 μmol/g, respectively. By comparing the adsorption behavior of functionalized MOFs, MIL-101(Fe)–NH 2 was proved to be most efficient for TCEP removal . Based on the adsorption experiments and DFT calculations, TCEP removal was dominated by physical adsorption. The van der Waals (vdW) interactions and hydrogen bonding were assumed to be involved in the adsorption. This work proves that appropriate ligand functionalization is promising for the removal of aqueous OPEs, which also provides a new insight for the control of OPEs pollution.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 10
·4806-4813
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IF 3.925
Jie Song,Leilei Sun,Hongchao Geng,Wenlong Tan,Deshuai Zhen,Qingyun Cai
β-Phase NaYF4:Yb,Tm,Gd up-conversion nanorods (UCNRs) with high uniformity were synthesized by a solvothermal method. The optimal fluorescence intensity of UCNRs was explored. After further modification with Materials of Institute Lavoisier-100(Fe) (MIL-100(Fe)) by the layer-by-layer self-assembly method, near-infrared light-triggered UCNR@MIL-100(Fe) nanomaterials with excellent antibacterial performances were constructed. A core–shell structure was constructed and confirmed by transmission electron microscopy (TEM). Reactive oxidizing species (ROS) detection indicated that the nanomaterials owned good photodynamic efficacy. The antibacterial experiments showed that the nanomaterials with 980 nm light irradiation and hydrogen peroxide (H2O2) had good antibacterial activity against Gram-negative and Gram-positive bacteria. Under 980 nm laser excitation, UCNRs generated ultraviolet and visible light to activate MIL-100(Fe) and induced a photo-Fenton reaction, which further produced oxygen species for antibacterial applications.
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ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Yue Hu,Zhou Fang,Xinyi Wan,Xu Ma,Yuqi Wang,Mengyang Dong,Zhizhen Ye,Xinsheng Peng
Developing efficient water adsorbents for solar-driven atmospheric water harvesting (AWH) still remains a challenge due to the poor photothermal heating ability and slow sorption kinetics of most adsorbents. Postsynthetic ligand exchange (LE) provides an alternative strategy to prepare metal–organic framework (MOF) materials with varied structures and functions. In this work, multifunctional hollow MIL-101(Cr) with ferrocene dicarboxylic acid (Fc(COOH)2) ligand exchanged (HMF) nanospheres are prepared and utilized for efficient AWH. The resulted HMF nanospheres present great visible light absorption (>80%) and photothermal conversion ability (61.6%) due to the introduced Fc(COOH)2 ligand. The water adsorption and desorption rates of the HMF nanosorbent are 2.3 times and 4.5 times that of MIL-101(Cr). The fast water capture and solar-driven release kinetics of HMF nanosorbents indicate its great potential for actual water harvesting. The outdoor water collection experiment demonstrates that the areal water harvesting capacity of the HMF nanosorbent is 1720 g m–2 per cycle with packed thickness of 8 mm. HMF nanosorbents also demonstrate good antibacterial activity (91.4%), which is beneficial to the collection of healthy and safe water. This work provides a facile and practical method to design multifunctional MOFs from the molecular level by LE and to achieve solar-driven AWH and other fields.
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Journal of Cleaner Production
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2022
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IF 11.072
Linxuan Xie,Tianshu Zhang,Xinyu Wang,Wenxin Zhu,Zhaoli Liu,Manshun Liu,Jing Wang,Liang Zhang,Ting Du,Chengyuan Yang,Mingqiang Zhu,Jianlong Wang
Semiconductor-based photocatalyst , whose efficiency distinctly hinges on the separation of photoinduced charge transfer within the interface of bulk structure, has incurred some intractable issues due to the existing energy barrier. Regulating the structure of MOF reasonably would feature an accelerated charge separation, and an effective utilization of photogenerated charges. Herein, a new type of MOF with both interior linker and metal valence modulation (m-MIL-101–1.0) is reported to boost photocatalytic activity owing to the formed charge migration pathway. At first, we introduced defective sites via CTAB, which acted as exposed sites for further reduction reaction. Then, NaBH 4 was used to achieve metal valence regulation. Benefiting from the unique structure, the Fe 3+ /Fe 2+ redox center was considered as a driving force to facilitate the charge transfer. It is properly considered that the activity improvement is attributed to the synergistic effect of both internal and external charge transfer channels. As a result, such m-MIL-101–1.0 has a higher activity than that of MIL-101 for photocatalytic degradation of tetracycline in water. We envision this interior configuration would be an ideal paradigm for tuning the activity of MOFs and extending the boundaries of MOF-based photocatalysts.
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Molecular Catalysis
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2022
·
IF 5.089
Cong Wang,Gang Li,Hongchen Guo
Compared with the mainstream approaches of doping the active metal in the MOFs structure and post-synthetic modification, it is more convenient to directly use the coordinatively unsaturated metal sites of MOFs for catalytic reactions. Herein, two forms of Ni-MIL-77 (1D Ni-MIL-77 and 3D MIL-77) were prepared using one-pot method and characterized by ICP-AES, XRD, FT-IR, XPS and SEM. Among them, 1D Ni-MIL-77 without high temperature heat treatment exhibited a better heterogeneous catalytic ethylene dimerization activity that was up to 989.6 g pro. /(g cat. ·h) (TOF=5544 h −1 ) and the selectivity of 1-butene could reach 93.3% at the optimal conditions. In addition, a probable Cossee-Arlman-like mechanism was proposed. By studying the catalyst structure after reaction, it was found that the reason for limited reuse was the hydrolysis products of the co-catalyst covered the catalysts.
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Materials
·
2022
·Vol. 15
·期 16
·5763
·
IF 3.748
Minmin Zou,Hexin Zhu,Ming Dong,Tian Zhao
As one of the most important prototypical chromium-based MOFs, MIL-101(Cr) is well-studied and widely employed in various scientific fields. However, due to its small capture window sizes and curved internal apertures, its application in large molecular removal is quite limited, and given its high stability and high synthetic temperature (>200 °C), it is difficult to achieve hierarchically porous MIL-101(Cr). In our study, hierarchically porous MIL-101(Cr) involving a high macro-/meso-/micropores ratio was designed and synthesized using acetic acid as an additive and silicon dioxide (SiO2) nanoparticles as a template. The optimal hierarchically porous MIL-101(Cr) (A-4) possessed a high specific surface area (2693 m2g−1) and an abundant macro-/mesoporous structure with the addition of SiO2of 200 mg. Compared with the control sample (A-0) with a less macro-/mesoporous structure, A-4 showed good adsorption properties for both coomassie brilliant blue R-250 (CBB, 82.1 mg g−1) and methylene blue (MB, 34.3 mg g−1) dyes, which were 1.36 times and 9.37 times higher than those of A-0. Moreover, A-4 also had good recyclability, and the removal rate of CBB was still higher than 85% after five cycles of adsorption.Keywords:MIL-101(Cr);SiO2;dye adsorption;template
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PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Liwei Sun,Meilin Yin,Zhen Li,Shaokun Tang
To alleviate environment issues derived from CO 2 emission, developing effective and economical methods for CO 2 capture has attracted much attention for decades. Metal-organic frameworks possess high porosity and stability, which is favorable to the adsorption of small molecules. Herein, an aluminum-based MOF, aluminum terephthalate [MIL-53(Al)], was synthesized with H 2 O and N , N′ -dimethylformamide as co-solvent via microwave-assisted method for CO 2 adsorption. The parameters including pre-mixing mode, microwave temperature, microwave power and reaction time were varied to study their influences on crystal structure, morphology and CO 2 adsorption capacity of MW-MIL-53(Al). Wherein, MW-MIL-53(Al) prepared with pre-mixing mode of stirring at 130 °C, 200 W and 3 h presents high crystallinity and rod-like morphology. The synthesized MW-MIL-53(Al) possesses relatively high BET surface area (961 m 2 /g), pore volume (0.46 cm 3 /g) and thermal stability (up to 480 °C), and its CO 2 adsorption capacity is 2.16 mmol CO 2 /g adsorbent under 25 °C and 0.1 MPa, which is higher than CS-MIL-53(Al) synthesized via conventional solvothermal method at 130 °C for 48 h.
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Energies
·
2022
·Vol. 15
·期 16
·5851
·
IF 3.252
Yong Yao,Shizhu Li,Chuangting Chen,Dongchen Zheng,Zhichao Wu,Chi Yu,Shuying Pu,Fa-Qian Liu
MIL-53(Fe) was prepared and modified with benzoic acid to prepare MIL-53(Fe)-BA additive, which was used to improve the catalytic oxidation rate of sulfite, prevent the scaling of the desulfurization tower, and improve the desulfurization efficiency during the wet flue gas desulfurization (WFGD) process of power plants. MIL-53(Fe)-BA exhibits abundant Lewis acid sites because of the appearance of coordination unsaturated Fe atoms. Due to the excellent sorption capacity, Ca(OH)2was used as the main SO2desulfurizer. The composite desulfurizers were prepared by mixing MIL-53(Fe)-based additives and Ca(OH)2, and were characterized by SEM, XRD, and FT-IR. A desulfurization unit was set up at laboratory scale to study the effect of catalytic oxidation additives on sulfite oxidation and desulfurization efficiency. The results showed that the addition of MIL-53(Fe)-BA can increase the oxidation capacity of sulfite by 159%, and greatly improve the desulfurization efficiency. These composite desulfurizers broaden the adaptability of the desulfurizing system to high-sulfur coals, and provide support for improving the desulfurizing efficiency of power plants.Keywords:catalytic oxidation;oxidative desulfurization;wet flue gas desulfurization;calcium hydroxide;MIL-53(Fe);Lewis acid sites
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Environmental Science-Nano
·
2022
·Vol. 9
·期 8
·3081-3093
·
IF 9.473
Yuqi Wan,Huaizhi Yang,Qigao Shang,Qingrong Cheng,Hong Zhou,Zhiquan Pan
A novel metal–organic framework@covalent organic framework (MOF@COF) heterojunction was synthesized based on post-synthetic covalent modification. In the present work, aldehyde-modified MOFs (NH2–MIL-101(Fe)) were covalently bonded with covalent organic frameworks (Schiff base network-1, SNW-1) forming the NH2–MIL-101(Fe)@SNW-1 (MS-x) heterojunction by using this strategy. The MS-x heterojunction showed excellent photodegradation ability for pollutants and photocatalytic hydrogen production under simulated sunlight. The superior photocatalytic performance of the MS-x heterojunction can be attributed to the formation of –CN– bonds between NH2–MIL-101(Fe) and SNW-1, which enhances the charge separation efficiency and improves the stability of the photocatalyst. It is worth mentioning that SNW-1 on the surface of the catalyst had a hollow structure which can promote the photoelectric charge migration. Furthermore, the results verified that the matched band structure of NH2–MIL-101(Fe) and SNW-1 could induce a type II heterojunction, which could well explain the improved photocatalytic performance of the photocatalytic system. This work not only provides a new idea to construct highly efficient and stable MOF@COF heterojunctions but also broadens the applications of COF-based materials.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2022
·
IF 3.428
Zihao Hu,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
MIL-101(Fe)/Co 3 O 4 composites were synthesized using a facile solvothermal method to establish the superiority of a heterogeneous photochemical catalysis system in the presence of Na 2 S 2 O 8 with visible light irradiation. In the present system, the MIL-101(Fe)/Co 3 O 4 catalyst showed better catalytic performance than the single photocatalytic or chemical catalytic system, implying that the MIL-101(Fe)/Co 3 O 4 catalyst can combine both photocatalysis and chemical catalysis well. When tetracycline (TC) is the target pollutant, the highest degradation efficiency can be achieved within 40 min, reaching to 86 %. Crystallinity, morphology, and elemental valence of the MIL-101(Fe)/Co 3 O 4 composite were explored by using X-ray diffraction (XRD), scanning electron microscopy (SEM) as well as X-ray photoelectron spectroscopy (XPS). From the quenching experiments, it was found that 1 O 2 , SO 4 ‾, OH, and O 2 ‾ make contributions to the effective removal of tetracycline. Apart from that, the recovery and reuse characteristics of MIL-101(Fe)/Co 3 O 4 may facilitate the sustainable wastewater treatment.
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International Journal of Applied Ceramic Technology
·
2022
·Vol. 20
·期 1
·24-38
·
IF 2.328
Cong Zhou,HaiPeng Feng,GuangAo Liu,Feng Tao,Qi Liu
SiFeCO ceramic nanocomposites with porous structure have been successfully prepared via pyrolysis of novel iron-containing precursors, which were synthesized by modification of polycarbosilane with different contents of MIL-101(Fe), a kind of metal-organic framework made by our laboratory. Iron-containing precursors were pyrolyzed at relatively low temperatures ranging from 500 to 900°C under nitrogen atmosphere, the polymer-to-ceramic conversion process were investigated by Fourier transform infrared spectroscopy, X-ray diffraction (XRD), and thermo gravimetric analysis (TGA) measurements. SiFeCO ceramics with different iron contents were intensively studied with respect to their crystallization behavior, microstructure evolution, and porous morphology influenced by additive amount of MIL-101(Fe). The results of XRD and Transmission electron microscopy revealed that MIL-101(Fe)-modified precursors converted into amorphous SiFeCO ceramics when pyrolyzed below 700°C under nitrogen, extremely small Fe 3 O 4 and α-Fe crystallites with grain size of only 2–5 nm were in situ generated and dispersed uniformly in the SiCO ceramic matrix. Simultaneously, interconnected porous structure was created in the matrix by the decomposition of MIL-101(Fe). The as-obtained SiFeCO ceramics could serve as heterogeneous Fenton-like catalysts for the degradation of xylene orange and exhibit outstanding catalytic properties.
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