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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Adenosine-functionalized UiO-66-NH2 to efficiently remove Pb(II) and Cr(VI) from aqueous solution: Thermodynamics, kinetics and isothermal adsorption

Hao Wang,Shuai Wang,Shixing Wang,Jiali Tang,Yingbi Chen,Libo Zhang

A new zirconium-based adsorption material (UiO-66-AMP) was prepared by modifying UiO-66-NH 2 with 5-adenosine to effectively remove Pb(II) and Cr(VI) from wastewater. The SEM, EDS, XRS and FT-IR characterization confirmed the successful synthesis of UiO-66-AMP. We conducted a sets of experiments to test the adsorption effectiveness of UiO-66-AMP for Pb(II) and Cr(VI). The maximum adsorption capacity of UiO-66-AMP for Cr(VI) (pH=2) and Pb(II) (pH=4) are 196.60 and 189.69 mg/g, respectively. The adsorption process conforms to the pseudo-second-order and Langmuir models, which indicates that the adsorption is a single-layer chemical process. Gibbs free energy ( ∆G) indicates that the adsorption of Pb(II) is an exothermic reaction , while the adsorption of Cr(VI) is an endothermic reaction . At the same time, the adsorbent maintains excellent adsorption capacity at least after 4 cycles. The good adsorption performance of UiO-66-AMP towards the metal ions was attributed to the surface complexation and electrostatic interactions. Therefore, the new adsorbent has obvious application prospect to remove Pb(II) and Cr(VI) from wastewater.

CAS / MDL: 10312-55-7 68-12-2
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MICROCHIMICA ACTA · 2023 ·Vol. 190 ·期 11 ·1-11 · IF 5.7

Ionic liquid-modified UiO-66-NH2 as sorbent of dispersive solid-phase extraction for rapid adsorption and enrichment of benzoylurea insecticides

Li Dan,Gao Yanmei,Mu Mengyao,Zhu Shiping,Zhang Ning,Lu Minghua

Ionic liquid (IL)-modified UiO-66-NH 2 composite was prepared and used as sorbent of dispersed solid-phase extraction (dSPE) for extracting trace benzoylurea insecticides (BUs) from complex environmental matrices. The IL in framework endowed the prepared material had electropositive characteristics, which can produce interaction with electron rich guest molecules, such as BUs. The high thermal and chemical stability of UiO-66-NH 2 /IL enabled it to be reused for 16 times without significant reduction in adsorption performance. Due to the multiple forces including π-π, hydrogen bonding, and fluorine-fluorine interaction, UiO-66-NH 2 /IL showed good adsorption performance, short adsorption time (20 s) and rapid desorption ability (60 s) for BUs. Under the optimal conditions, the method exhibited wide linear range (0.02–500 ng mL -1 ) with correlation coefficient ( R 2 ) not worse than 0.9928, high enrichment factor (252–300), and low detection limit (0.005–0.4 ng mL -1 ). The dispersed solid phase extraction coupling with high-performance liquid chromatography-diode array detector (dSPE-HPLC-DAD) was successfully used to detection of BUs in real environmental samples and satisfactory recoveries were obtained (80.5%±2.4–118%±3.2). The results indicated that UiO-66-NH 2 /IL composite can be a potential sorbent for the preconcentration of trace insecticides in environmental samples. Graphical abstract

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JOURNAL OF SOLID STATE CHEMISTRY · 2023 · IF 3.3

Post-synthetic modification of NH2-MIL-101(Al)@SiO2 with different non-polar ligands for improving HPLC separation performance of estrogens

Rui Zhao,Cheng Cheng,Xiurong Wu,Xueyan Bai,Fenghuan Wang

Due to the excellent pore structure , MOFs as the stationary phase was playing an important part in chromatography . In this work, the shell-core MIL-101(Al)@SiO 2 composites post-synthetic modified by ligands with different polarities were fabricated for separation of estrogens. The structure and morphology of these materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), scanning electron microscope (SEM) and Brunauer-Emmett-Teller (BET). In order to investigate the influence of the ligand polarity on chromatographic separation performance of estrogens, alkyl molecules with different chain length were introduced as the ligands. With the hydrophobicity and chain length of the ligands increasing, the resolutions of the MIL-101(Al)@SiO 2 columns for the separation of estrogens exhibited the tendency of a parabola. Best result was achieved on the C4-MIL-101(Al)@SiO 2 column. On that basis, the possible retention mechanism on C4-MIL-101(Al)@SiO 2 column was elucidated by studying the mobile phase effect on separation behavior.

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Journal of Environmental Chemical Engineering · 2020 · IF 4.3

Removal of Ca2+ and Mg2+ from oilfield wastewater using reusable PEG/Fe3O4/GO-NH2 nanoadsorbents and its efficiency for oil recovery

Lei He,Lutao Yang,Luxia Zhang,Zhe Wang,Hongjie Cheng,Xiaoguang Wang,Jianrong Lv,Jun Zhang,Hong Mo,Jian Shen

The high salinity of oilfield-produced water caused by the presence of metal ions, such as Ca 2+ and Mg 2+ , has a significantly adverse effect on oil recovery. It is crucial to remove these metal ions efficiently before the oilfield wastewater is reinjected down into the oil wells. To address this issue, we prepared a PEG/Fe 3 O 4 /GO-NH 2 nanoadsorbent by aminating GO, incorporating magnetic Fe 3 O 4 nanoparticles and coating with PEG (PEG = poly(ethylene glycol); GO-NH 2 = aminated graphene oxide). We investigated the removal ratios of the nanoadsorbent for Ca 2+ and Mg 2+ . The respective removal ratios for Ca 2+ and Mg 2+ reached 69.8 % and 61.1 % at 10 min, indicating that the nanoadsorbent was capable of efficiently removing Ca 2+ and Mg 2+ . We also evaluated the reusability of the nanoadsorbent by recycling and reusing it 5 times. At the fifth recycling run, the nanoadsorbent retained relatively high reuse rates (79.1 % for Ca 2+ , 69.5 % for Mg 2+ ) and removal ratios (69.5 % for Ca 2+ , 64.3 % for Mg 2+ ), suggesting that the nanoadsorbent possessed relatively high reusability. Oilfield wastewater treated with the nanoadsorbent was employed for oil recovery in core displacement experiments. The oil recovery efficiency significantly increased by 11.8 % compared with untreated oilfield wastewater. Therefore, the PEG/Fe 3 O 4 /GO-NH 2 nanoadsorbent exhibits considerable potential for the treatment of oilfield wastewater to enhance oil recovery.

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Energy Technology · 2020 ·Vol. 9 ·期 2 ·2000957 · IF 3.404

Carbon-Based Printable Perovskite Solar Cells with a Mesoporous TiO2 Electron Transporting Layer Derived from Metal–Organic Framework NH2-MIL-125

Bo Li,Jianhong Zhao,Qingjie Lu,Shiqiang Zhou,Haitang Wei,Tianping Lv,Yumin Zhang,Jin Zhang,Qingju Liu

Applying metal–organic framework (MOF) materials to perovskite solar cells (PSCs) is an innovative and promising direction in the current photovoltaic field, especially in low-cost carbon-based PSCs without hole transport layer. Herein, a novel mesoporous anatase TiO 2 nanocrystalline with pie morphology, large specific surface area (SSA), and outstanding wettability is successfully prepared by sintering the NH 2 -MIL-125 at 500 °C for 6 h. The TiO 2 derived from NH 2 -MIL-125 possesses excellent penetration and crystallinity of perovskite in the electron transporting layer (ETL), and exhibits appropriate work function which matches relatively better with the conduction band of perovskite. Meanwhile, the power conversion efficiencies (PCEs) of the two PSC devices based on the as-prepared TiO 2 are 13.49% and 12.55%, respectively. Moreover, both of these devices exhibit good stability.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

A novel strategy for enhancing the performance of membranes for dyes separation: Embedding PAA@UiO-66-NH2 between graphene oxide sheets

Haojie Zeng,Zongxue Yu,Liangyan Shao,Xiuhui Li,Meng Zhu,Yuchuan Liu,Xiaofang Feng,Ximei Zhu

A composite membrane based on a novel strategy was prepared which using graphene oxide (GO), UiO-66-NH 2 and polyacrylic acid (PAA) as basic materials on the surface of nylon membrane by vacuum filtration self-assembly. The structure of the composite membrane was made of graphene oxide as vertical separation layer, the PAA@UiO-66-NH 2 (PAA@UiO) embedding between GO as horizontal capture material. The PAA@UiO-66-NH 2 /GO (PAA@UiO/GO) membrane was characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and atomic force microscopy (AFM). Compared with the GO membrane, PAA@UiO/GO membrane combined the effects of GO, UiO-66-NH 2 and PAA, which significantly enhances the separation performance of dye wastewater. In particular, the PAA@UiO/GO membrane can achieve complete removal of MB , RB and CR while the fluxes during filtration process can reach about 100  L ∙ m - 2 ∙ h - 1 . At the same time, PAA@UiO/GO membrane almost retained stable removal rate on all dyes under extreme pH and ionic strength conditions. In addition, after 10 cycles of experiments, PAA@UiO/GO membrane retained a removal rate and a flux more than 95% and 85  L ∙ m - 2 ∙ h - 1 for all dyes, respectively. Compared to a composite membrane based on intercalation, the unique structure of PAA@UiO/GO membrane with a large number of adsorption sites and screening structures, resulting a better removal rate for dyes. Furthermore, PAA@UiO/GO membrane has a great potential in practical applications and a solution to balance trade-off effect.

CAS / MDL: 7782-42-5 9003-01-4
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Defect engineering of NH2-MIL-88B(Fe) using different monodentate ligands for enhancement of photo-Fenton catalytic performance of acetamiprid degradation

Yuexin Wang,Zhen Zhong,Yaseen Muhammad,Hui He,Zhongxing Zhao,Shuangxi Nie,Zhenxia Zhao

Engineering of monodentate ligands induced defects was proposed to modify NH 2 -MIL-88B(Fe) in order to promote its synergetic photo-Fenton catalytic degradation performance for acetamiprid (ACTM) as model neonicotinoid insecticides. Three monodentate ligands with different coordination groups (benzoic acid, pyrrole and pyrrole-2-carboxylic acid) were applied to in-situ induce ligand vacancies on NH 2 -MIL-88B(Fe). Effect of defect coordination mode on its photo-Fenton catalytic performance was investigated through the ACTM degradation reaction. Ligand defects on NH 2 -MIL-88B(Fe) would generate three merits: (1) it can modulate surface properties to enhance adsorption affinity towards ACTM; (2) it can introduce large amount of monodentate ligands and ligand vacancies in MOFs to promote light absorption and electron-hole separation capacity for photo-catalysis; (3) it can increase the amount of Fe Lewis acid sites to improve redox capacity of Fe 2+ /Fe 3+ for Fenton-catalysis. In this work, Pyrrole-2-carboxylic acid (Pac) was proved to introduce more monodentate ligands in MOFs and generate more ligand vacancies as well. As a result, ACTM can be easily captured by defective NH 2 -MIL-88B(Fe) and degraded by in-situ triggered oxidative reaction through the synergistic “photo-Fenton catalysis”. Performance measurements showed that Pac-MIL88(Fe) achieved 7.3 times higher adsorption rate and 5.5 times higher catalytic rate for ACTM than that of pristine MIL88(Fe). Moreover, total organic carbon (TOC) conversion reached 97.0% within only 90 min using Pac-MIL88(Fe) as photo-Fenton catalyst, showing 1.7 times higher than pristine MIL88(Fe). Thus, the in-situ fabrication of ligand defect-containing MIL88(Fe) can be foreseen of potential for designing new MOFs for wider practical applications.

CAS / MDL: 109-97-7
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CELLULOSE · 2019 ·Vol. 26 ·期 17 ·9335-9348 · IF 3.917

Robust fluorine-free colorful superhydrophobic PDMS/NH2-MIL-125(Ti)@cotton fabrics for improved ultraviolet resistance and efficient oil–water separation

Yang Yingying,Huang Wei,Guo Zengpei,Zhang Shiyu,Wu Feng,Huang Jingjing,Yang Hongjun,Zhou Yingshan,Xu Weilin,Gu Shaojin

Abstract Superhydrophobic cotton fabrics with improved ultraviolet resistance were prepared via in situ growing NH 2 -MIL-125(Ti)(Ti-MOF) nanoparticles on cotton fibers and subsequently coating with polydimethylsiloxane (PDMS) under room temperature. The synergetic effect of Ti-MOFs nanoparticles and PDMS was critical and essential for obtaining a superhydrophobic coating with anti-UV property. The surface microstructure, chemical composition, and superhydrophobic property of the as-prepared fabrics were characterized by K/S value, scanning electron microscopy, X-ray photoelectron spectroscopy, energy dispersive spectroscopy, and water contact angle (WCA) measurements. The as-prepared cotton fabrics not merely exhibited desirable superhydrophobic property with a water contact angle (WCA) of 154.7 ± 0.7° and a sliding angle of 3.6°, but also displayed the considerable UV resistance. The oil–water separation, stability of UV protection and superhydrophobicity were also investigated. The superhydrophobicity, anti-ultraviolet property, and K/S value of as-prepared PDMS/Ti-MOFs@cotton fabrics were stable after 300 cycles of abrasion and 5 cycles of washing. The facile synthesis technique provided a simple method for scalable construction of multifunctional fabrics. Graphic abstract

CAS / MDL: 10312-55-7 546-68-9
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Post-functionalization of UiO-66-NH2 by 2,5-Dimercapto-1,3,4-thiadiazole for the high efficient removal of Hg(II) in water

Likang Fu,Shixing Wang,Guo Lin,Libo Zhang,Qiming Liu,Ju Fang,Chenhuinan Wei,Gang Liu

A new MOFs adsorbent was prepared by post-functionalization of UiO-66-NH 2 with 2,5-Dimercapto-1,3,4-thiadiazole and utilized to remove the Hg(II) in water selectively. The UiO-66-types were detected by Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscope (FESEM), Brunauer-Emmett-Teller (BET) and zeta potential instruments. The adsorption properties of the new MOFs adsorbent were investigated by batch experiments. The actual maximum adsorption amount was 670.5 mg/g at the optimal pH of 3. Adsorption kinetic and isotherm models were exceedingly fitted to pseudo-second-order and Langmuir/Dubinin-Radushkevich, respectively. The adsorption process and mode were geared to monolayer and chemisorption, the removal rate was directly proportional to the square of mercury ions concentration. The UiO-66-DMTD adsorbent was easy to be regenerated and the removal rate decreased by only 13.5% after ten consecutive cycles. The results of FTIR, XRD and XPS suggested that the adsorption mechanism lay on the complexation reaction between Hg(II) and thiol/nitrogen-containing groups. Moreover, compared with other competitive metal ions, viz., Zn(II), Co(IV), Ni(II), Cd(II), Mg(II), Fe(III), Ca(II) and Cu(II), the UiO-66-DMTD demonstrated an outstanding selective adsorption for Hg(II). These results manifested that the UiO-66-DMTD was a latent adsorbent for the efficient and selective removal of Hg(II) in wastewater.

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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Simple fabrication of flake-like NH2-MIL-53(Cr) and its application as an electrochemical sensor for the detection of Pb2+

Hongxu Guo,Dongfang Wang,Jianhua Chen,Wen Weng,Minqiang Huang,Zishan Zheng

A novel metal-organic framework (MOF) material, flake-like NH 2 -MIL-53(Cr), was prepared by a simple reflux method and then characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). The as-prepared MOF was found to be an effective material for the selective electrochemical detection of microgram levels of Pb 2+ in aqueous solution. Detection was performed by square wave anodic stripping voltammetry. The NH 2 -MIL-53(Cr)-modified electrode showed excellent selectivity and stability for Pb 2+ detection. The electrochemical properties and applications of the modified electrode were studied. Operational parameters such as pH, deposition potential, and deposition time, were also optimized to detect trace amounts of metal ions. This method offers a new strategy for heavy metal detection using MOF materials.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2017 · IF 9.446

Palladium-decorated hierarchical titania constructed from the metal-organic frameworks NH2-MIL-125(Ti) as a robust photocatalyst for hydrogen evolution

Baolin Yan,Lijuan Zhang,Zhiyong Tang,Mohammad Al-Mamun,Huijun Zhao,Xintai Su

Engineering metal-organic frameworks (MOFs) into hierarchical structured materials is crucial for providing a viable platform to construct efficient catalysts and broaden their applications in energy conversion and photocatalysis. Here, a simple and efficient solid-state pyrolysis of Ti-MOFs (NH 2 -MIL-125) sacrificial template combined with a photo-reduction process was developed to construct a series of hierarchical TiO 2 decorated with Pd nanoparticles. The hierarchical TiO 2 inherited the well-defined rounded rectangular submicron-tablet from NH 2 -MIL-125 precursor and was constituted of uniform anatase TiO 2 nanoparticles with an average size of 12   nm. Furthermore, the photocatalytic activity for the hydrogen production from water-methanol solution was improved by the optimization of the content of Pd as a cocatalyst, and the maximum was achieved with a Pd loading of 1.5%. The rate of H 2 evolution of 1.5% Pd decorated hierarchical TiO 2 (1.5% Pd/TiO 2 ) reached to 979.7   μmol   h −1 and 112.7   μmol   h −1 , under UV–vis light and simulated solar light, respectively. This unusual photocatalytic activity may be resulted from the positive synergetic effect of efficient light absorption, promoted separation and migration of photo-induced electron-hole carriers. The work highlights the potential of the MOFs-based hierarchical TiO 2 in the photocatalytic water splitting under solar light.

CAS / MDL: 7647-10-1 3087-37-4
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Direct Z-scheme charge transfer Bi2O3/UiO-66-NH2 heterojunctions for boosted photocatalytic degradation of tetracycline hydrochloride in different water systems

Shipeng Liao,Muhammad Arif,Xingyue Qian,Guangyu He

The development of hybrid heterostructure photocatalysts with enhanced visible light absorption capacity holds significant importance in environmental remediation. However, the challenge persists in exploiting strong visible-light responsive photocatalysts with both high efficiency and stability. Herein, we successfully synthesized a hybrid Z-scheme heterojunction of Bi 2 O 3 and UiO-66-NH 2 (Bi 2 O 3 /UiO-66-NH 2 ) through a simple hydrothermal route. The visible light photocatalytic performance of Z-scheme Bi 2 O 3 /UiO-66-NH 2 heterojunction is systematically evaluated for persistent antibiotic tetracycline hydrochloride (TC-HCl) both in the clean and real water matrix. All heterojunction catalysts exhibit superior photodegradation capabilities compared to pristine Bi 2 O 3 and UiO-66-NH 2 . The optimal ratio of the two components heterojunction (BUN-150), in particular, demonstrates the highest removal efficiencies for TC-HCl (95 %) within a 90-min timeframe. This remarkable photocatalytic performance is credited to the Z-scheme charge transfer occurring at the interface of Bi 2 O 3 and UiO-66-NH 2 in Bi 2 O 3 /UiO-66-NH 2 heterojunction. The active species experiments and electron paramagnetic resonance analyses are conducted to identify the active reactive species during the TC-HCl degradation (·OH, h + , and ·O 2 − ), and a precise photocatalytic degradation mechanism is explained. Additionally, the photodegradation intermediates of TC-HCl are detected using the HPLC-MS analysis to explain the degradation pathways of TC-HCl. This research paves the way for the development of novel Z-scheme Bi 2 O 3 -based heterojunction catalysts for outstanding photocatalytic applications.

CAS / MDL: 64-75-5
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