Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Yongtong Lei,Lijing Zhu,Jilong Xu,Shuan Liu,Zhixiang Zeng,Xiaocheng Li,Gang Wang
Metal organic framework (MOF) with fine pore structures, ultra-high porosity and large specific surface area can provide more water transport channels while achieving precise sieving of different sizes of ions, which is a promising material for high efficiency desalination. However, particle agglomeration, interface incompatibilities and interface defects severely restrict the performance of MOF-based membranes. It is still a challenge to construct MOF-based desalination membranes with both high water permeability and high ion sieving. Herein, the UiO-66-NH 2 based nanofiltration membrane was fabricated by in-situ growth of UiO-66-NH 2 on Nylon membrane and composed with polyamide (PA) layer by interfacial polymerization (IP). With 12 h solvothermal reaction, the UiO-66-NH 2 nanoparticles are found uniformly loaded on the Nylon substrate. Therefore, the water molecule transport channels provided by UiO-66-NH 2 nanoparticles reduce the transport resistance, which can improve the water permeability. More importantly, UiO-66-NH 2 nanoparticles are found to be involved in the IP process, which can reduce the interfacial defects and thus enhance the bonding force between the PA layer and base film. The synergistic effect of the UiO-66-NH 2 and PA layer improves the nanofiltration performance of the membrane with rejection rate of 92.97% for Na 2 SO 4 and the pure water permeance (PWP) of 11.55 L m −2 h −1 bar −1 . The N-UN12 @PA membrane also has excellent antifouling performance (flux recovery ratio (FRR) of 95.86%, reversible fouling ratio (Rr) of 33.93%, irreversible fouling ratio (Rir) of 4.14%). Unlike the mixed-matrix membrane (MMM) and polycrystalline MOF membrane, this strategy provides a promising method to prepare high-performance nanofiltration membrane for desalination.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Nian Li,Zi-jian He,Jia-hui Zhao,Zhi-dong Zhao,Xing-rui Qi,Hao-dong Wang,Bo Liu,Hua-jie Lai,Tao Jin
Developing magnetic adsorbent that combines the merits of quick response, excellent enrichment capacity, uniform and stable dispersivity is of paramount importance in pollutants pretreatment. In this work, tunable strawberry-like Fe 3 O 4 @SiO 2 -NH 2 @Au@ 2-ME magnetic solid phase extraction materials were prepared via assembly method. The obtained nanocomposites were characterized using scanning electron microscopy, X-ray diffraction spectroscopy, infrared spectroscopy , X-ray photoelectron spectroscopy, and whereafter the preparation method was optimized. Integrating magnetic solid-phase extraction with high-performance liquid chromatography and fluorescence detection , a comprehensive enrichment and detection method toward bisphenol A (BPA) was well established. This method demonstrated high efficiency and rapidity, achieving rapid enrichment of BPA. The as-developed method exhibited good linear correlation within the range of 10.0–500 μg·L −1 , with a recovery of 85–92%. It showed excellent sensitivity and reproducibility in BPA extraction with low limit of detection (LOD, 0.274 μg·L −1 ), limit of quantitation (LOQ, 0.913 μg·L −1 ) and relative standard deviation (RSD, 1.5%, n = 6), respectively. The proposed Fe 3 O 4 @SiO 2 -NH 2 @Au nanoplatform firmly supports the envision that proper surface functionalization of magnetic substrate could promote the enrichment capacity toward various pollutants in actual application scenarios.
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Journal of Environmental Chemical Engineering
·
2020
·
IF 4.3
Yi Cheng,Jilin Zhang
Excessive phosphate in wastewater can cause eutrophication of water body, which will worsen the ecological environment and threaten human health and biological life safety. Adsorption of phosphate is the most effective way to remove phosphate, and efficient adsorbent is the key. Amorphous La(OH) 3 has been deemed as a potential phosphate adsorbent on account of high adsorption capacity and environmentally friendly property. However, it also shows some disadvantages such as easy agglomeration, poor water dispersion. In this study, UiO-66-NH 2 was used as carrier to load amorphous lanthanum hydroxide as an adsorbent for phosphate removal. The adsorbent (UiO-66-NH 2 @La(OH) 3 , ULCs) has good water dispersibility and it is easy to be separated and recovered. At the same time, the maximum phosphate adsorption capacity can reach 140.7 mg P/g. The adsorption process accords with pseudo second order kinetic model and Freundlich isotherm model. The thermodynamic results showed that the adsorption process was spontaneous and endothermic. In addition, in the presence of coexisting anions (such as Cl − , SO 4 2− , NO 3 − ), it also exhibited high selectivity and phosphate removal efficiency. Meanwhile, the adsorption capacity keeps at a high level in the range of pH 3–11. By the merit of above-mentioned properties, the prepared material is expected to be an ideal candidate for phosphate removal from contaminated water.
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Catalysts
·
2020
·Vol. 11
·期 1
·24
·
IF 3.52
Juan Du,Jiaxin Zhang,Tingyu Yang,Renming Liu,Zhiyi Li,Dandan Wang,Tong Zhou,Yucun Liu,Chunbo Liu,Guangbo Che
The BiOI/NH2-MIL-125(Ti) composite photocatalyst with excellent photocatalytic performance was prepared by the solvothermal method. For the BiOI/NH2-MIL-125(Ti) (BNMT) system, the contents of NH2-MIL-125(Ti) in BNMT-4, BNMT-5, BNMT-7, BNMT-9, and BNMT-10 were 4 wt %, 5 wt %, 7 wt %, 9 wt %, and 10 wt %, respectively. XRD, XPS, SEM, and TEM characterizations indicated that BiOI/NH2-MIL-125(Ti) was successfully prepared. Brunauer, Emmett, and Teller (BET) and UV–vis diffuse reflectance spectra photoelectrochemical analysis indicated that BNMT-9 can make the specific surface area and photo absorption region larger than BiOI. In addition, the separation efficiency of photogenerated carriers was improved, and the recombination efficiency was reduced. The degradation percentages of Rhodamine B (RhB) and p-chlorophenol (P-CP) reached 99% and 90% over BNMT-9 under visible light irradiation. Additionally, the catalysts had high stability. The results of the active spices trapping experiments test indicated that h+was the main active species. The possible degradation mechanism was proposed.Keywords:photocatalysis;BiOI;NH2-MIL-125(Ti);organic pollutants
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2020
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IF 3.232
Chunhua Lin,Zhifeng Zou,Zhiwei Lei,Li Wang,Yonghai Song
Ellagic acid (EA) is a symmetric natural phenol bioactive compound present in fruits and nuts, and has attracted substantial interest worldwide owing to its beneficial health effects. Here, the exploration of luminescent metal-organic frameworks (MOFs) of MIL-101(Al)-NH 2 (MIL = Materials of Institute Lavoisier) for rapid and sensitive sensing of EA in aqueous solution was reported initially. The porous MIL-101(Al)-NH 2 MOFs was synthesized by solvent-thermal method with inexpensive 2-aminoterephthalic acid and aluminum salt, which exhibited uniform spherical crystals (~340 nm) and specific mesoporous structure (3.2 nm). The fluorescence intensity of MIL-101(Al)-NH 2 at 425 nm showed a good linear relationship with EA concentration in the range of 0.15–100 μM. The detection limit was as low as 43.8 nM, the rapid response time was within 2 min, and the cost of detection was low. In addition, the “turn off” fluorescence probe could be utilized for visual detection of EA according to the color change under the UV lamp. Based on the Stern-Volmer equation, the quenching constants was decreased with the rise of temperature, which indicated that the probable quenching mechanism was static quenching. The nanoprobe was successfully used to detect EA in the cherry and serum samples. MIL-101(Al)-NH 2 represents the first instance of MOFs-based fluorescent probe in EA detection. This work not only enriches the detection method of EA, but also expands the potential application of MIL MOFs in small molecules.
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Arabian Journal of Chemistry
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2020
·
IF 4.762
Zhen Huang,Chen Wang,Jiling Zhao,Shixing Wang,Yang Zhou,Libo Zhang
A new adsorbent was successfully fabricated by chemically linking pyromellitic acid onto a zirconium-based metal-organic framework composite for selective adsorption of Pd(II) from an aqueous solution. The adsorbent was characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller equation and scanning electron microscope. The adsorption capacity, selectivity and repeatability of the adsorbent were tested by batch experiments. The optimum pH was 2.0, and the maximum adsorption capacity at room temperature was 226.1 mg/g. In the kinetic experiments, the adsorption process achieved equilibrium within 5 h and generally conformed to the quasi-second kinetics and Freundlich isotherm model. The N-H and O H groups on the adsorbent interacted with Pd(II) by electrostatic and coordination action. The adsorbent maintained excellent adsorption capacity after at least 5 cycles. At the same time, the selectivity of the adsorbent in aqueous solution is excellent from interfering ions. Therefore, the new adsorbent will have an obvious application prospect on the recovery of palladium.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Ju Liu,Dandan Hao,Huiwen Sun,Yu Li,Jianlin Han,Bo Fu,Jiancheng Zhou
In this Article, a hybrid foam was fabricated through the integration of amine-functionalized Fe-MOF (MIL-101-NH2) into cellulosic matrix. The existence of enormous group linkages and ionic bonding interactions among the composite foam network leads to a uniform dispersion of MIL-101-NH2 and high affinity between the MOF and cellulose skeleton. As-prepared hybrid foams were utilized as photocatalysts to reduce toxic hexavalent chromium ions (Cr(VI)) under visible light. Optimal performance was observed over CM-1 (with a MIL-101-NH2 and nanocellulose mass ratio of 1:1). When compared to pure MOF nanoparticle counterparts, the CM-1 foam presented preferable and more efficient Cr(VI) removal performance. The reasons could be attributed to the hierarchal pore structure and uniform MOF loading. Moreover, the flexible foams could be easily separated from the solution and preserved more than 80% removal efficiency of Cr(VI) after 10 runs. This work would shed light on how to construct high-efficiency photocatalysts for environmental governance from sustainable materials.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 19
·6507-6515
·
IF 6.119
PanPan Xu,Liuxue Zhang,Xu Jia,Hao Wen,Xiulian Wang,Suqing Yang,Juxian Hui
Compared to the current commercial three-step production process involving low phenol yield, low atomic efficiency, and the formation of explosive intermediates, the direct oxidation of aromatic hydrocarbon to more desirable and important chemical industry intermediate such as phenol offers a more attractive and challenging pathway. Here, we report the selective photocatalytic hydroxylation of benzene to phenol using NH2-MIL-88/PMo10V2-3 as the catalyst and H2O2 as a mild oxidant. Heteropoly acid (PMo10V2) was immobilized to metal–organic frameworks (NH2-MIL-88), where PA anions play an essential role in anchoring NH3+ cations to form stable heterogeneous photocatalysts. The reaction offered a high selectivity of 99% with a yield of 24% for phenol under optimum reaction conditions. Comprehensive characterizations and experiments disclosed a multistep reaction mechanism in which high dispersion of PMo10V2, the production of hydroxyl radical(˙OH) and the formation of V5+/V4+ redox pairs are responsible for the activity of the reaction in the presence of electrons (e−). The recycling experiments were essential in confirming the reusability of the catalyst, and FT-IR characterization analysis also proved the integrity of NH2-MIL-88/PMo10V2-3 after three cycles. This work provides potential applications in the green and highly efficient photocatalytic synthesis of other organic compounds and other environmental applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Guanglai Mo,Linxi Wang,Jianhong Luo
It is a challenge to achieve efficient photocatalytic activity of pure MOFs. Herein, the defective NH 2 -MIL-125(Ti) with adjustable linker vacancy level was successfully created by thermal treatment. The band gaps of samples decreased and the more Ti-O clusters on the surface of the samples can be achieved as the time of thermal treatment increased from 0 to 500 min, both of which facilitated the photocatalytic activity for the reduction of Cr(VI). Moreover, the ligands from the surface to the inside of the samples were successively decarboxylated, resulting in the declined specific surface area and the increased proportion of mesoporous and the defect level. The moderate defect level in NH 2 -MIL-125(Ti) can be obtained as the time of thermal treatment was 300 min, which facilitated the separation of photogenerated charges, contributing to the highest photocatalytic activity for reduction of Cr(VI), which was 9.2 times than that of the initial MOFs. However, the excessive linker vacancy defect level in NH 2 -MIL-125(Ti) may result in the seriously affected crystal structure and the retarded separation of photogenerated charges.
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DESALINATION
·
2019
·
IF 6.035
Liangliang Dong,Minghui Li,Shuo Zhang,Xuejian Si,Yunxiang Bai,Chunfang Zhang
Graphene oxide (GO)-based nanofiltration membranes, featuring well-ordered microscopic structure, well-defined 2D nanochannels and superior molecular sieving ability, have attracted sustained research interest in molecular and ionic separation. However, most of current GO laminar membrane have a poor water flux and high rejection of both dyes and salts, which is not suitable for the dye/salt mixture separation. Herein, we report a vacuum filtration strategy to fabricate GO/NH 2 -Fe 3 O 4 nanofiltration membranes with high water flux and excellent separation performance for dye/salts mixture by introducing NH 2 -Fe 3 O 4 . The NH 2 -Fe 3 O 4 is not only worked as the rigid spherical nanospacer to tune GO interlayer spacing but also as crosslinkers to improve the stability of GO membrane in water. FTIR, XRD , SEM , zeta potential and contact angle were applied to analyze the chemical composition and morphology of as-prepared membranes. The effect of intercalated NH 2 -Fe 3 O 4 nanoparticles on overall performance of the GO/NH 2 -Fe 3 O 4 membranes was systematically investigated. The resulted membrane with 8 wt% of NH 2 -Fe 3 O 4 loading has high water flux of up to 78 Lm − 2 h − 1 , which is 4.8 times higher than that of pure GO membrane. Moreover, such membrane also displays high congo red rejection (94%) and low NaCl rejection (~15%), rendering the membranes promising for dye/salt mixtures separation.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
·
IF 3.261
Lingling Wang,Penglun Zheng,Xuefei Zhou,Mingzhen Xu,Xiaobo Liu
Novel CdS/UiO-66-NH 2 heterojunction photocatalysts have been successfully fabricated via facile water bath deposition. Compared with the traditional preparation technology, such strategy introduces deionized water as solvent, reduces production cost and simplifies the fabrication process of the heterojunction photocatalyst. Characterizations indicate that CdS nanoparticles (NPs) are uniformly interspersed on the surface of UiO-66-NH 2 and the intimate contacted heterojunction interface is generated to prevent recombination of photogenerated charge carriers. CdS/UiO-66-NH 2 with a mass ratio of 1.5:1 (CdS: UiO-66-NH 2 ) exhibits the highest photocatalytic degradation rate for RhB of approximately 92.5% in 40 min and excellent photostability through four recycles. Furthermore, Photoluminescence (PL) spectra, UV–vis diffuse reflectance spectra (DRS), transient photocurrent, electrochemical impedance spectra (EIS), Nyquist plots and Mott-Schottky plots are applied to characterize the photoelectrochemical properties. The observably enhanced photocatalytic performance can be attributed to: 1) larger specific surface area, increased photocatalytic active sites, intimate contacted interface, 2) created n-n type heterojunction, and 3) rapid separation and transfer of photoexcited interfacial charges.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 33
·11705-11712
·
IF 4.099
Cong-Cong Shen,Ya-Nan Liu,Xin Wang,Xiao-Xiang Fang,Zhi-Wei Zhao,Nan Jiang,Liu-Bo Ma,Xiao Zhou,Tuck-Yun Cheang,An-Wu Xu
Metal–organic framework (MOF)-based materials possess numerous attractive characteristics; however, the application of MOF-based photocatalysts in the area of visible-light photocatalytic H2 evolution is still in its infancy. Herein, we develop a series of novel UiO-66-NH2-based composites with embedded NiO nanoparticles via solvothermal treatment and subsequent calcination. Their characterizations demonstrate intimate lattice-level contacts between UiO-66-NH2 photocatalysts and NiO nanoparticles. By optimizing each component, even without noble metal loading, the U6N-NiO-2 sample (the weight ratio of NiO to U6N-NiO-2 is theoretically calculated to be ca. 10 wt%) with 15 mg eosin Y as a sensitizer causes an enhanced H2 generation rate of 2561.32 μmol h−1 g−1 under visible-light irradiation using TEOA as a sacrificial reagent; furthermore, its corresponding quantum efficiency is as high as 6.4% at 420 nm. The H2 evolution activity of U6N-NiO-2 is about 5 times higher than that of the UiO-66-NH2 photocatalyst (denoted as U6N) and 23 times higher than that of U6N-NiO-2 without sensitizer. It is demonstrated that the high efficiency originates from the visible-light generated electrons of eosin Y and UiO-66-NH2, the efficient separation of carriers by the cascaded band structure and more negative CB of NiO as well as the good dispersion of NiO nanoparticles on the octahedral skeleton. This study provides new insights for the design of MOF-based materials without noble metal loading for visible-light photocatalytic H2 evolution.
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