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NH2-UIO-66
ECS Journal of Solid State Science and Technology · 2024 ·Vol. 13 ·期 5 ·057004 · IF 1.8

Fluorescein@NH2-UiO-66 Probe for Ratiometric Fluorescence Sensing of Trace Phosphate in Water

Yu Ding,Yaru Li,Soufian Chakir,Jun Mei,Xianbiao Wang

Phosphate pollution leads to deterioration in water quality, posing a serious threat to human health. Therefore, it is important to develop a highly selective and sensitive fluorescent probe for phosphate detection. Here, we report a novel ratiometric fluorescent probe, Fluorescein@NH2-UiO-66 (denoted as Flu@NH2-UiO-66), for the trace detection of phosphate in water. Specifically, during the in situ solvothermal synthesis of Flu@NH2-UiO-66, fluorescein molecules were encapsulated into the cavities of the metal-organic framework. Furthermore, the encapsulation amount of fluorescein was controlled by adjusting the acidity of the system. The Flu@NH2-UiO-66 (60 H+) sample, prepared with a 60:1 molar ratio of acetic acid to the metal center exhibited distinct dual fluorescence signal peaks. The probe showed a highly selective fluorescence response to phosphate. Within a range of 0–20 μM phosphate concentration, the probe demonstrated excellent linear detection capability with a detection limit of 0.37 μM. Moreover, the mechanism of fluorescence enhancement can be attributed to the addition of phosphate, which greatly increases the UV absorbance of the probe. This study developed a novel ratiometric fluorescent probe capable of rapid, sensitive, and stable detection of trace phosphate, which is of great significance for environmental management.

研究领域: 环境科学 · 分析化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Polyethyleneimine NH2-UiO-66 nanofiller-based mixed matrix membranes for natural gas purification

Yuchen Cui,Xiaolei Cui,Lubomira Tosheva,Chunzheng Wang,Yongming Chai,Zixi Kang,Qiang Gao,Kun Wang,Zhihan Zhang,Hailing Guo,Daohong Xia,Daofeng Sun

Effective separation of CO 2 from CH 4 is crucial for the purification of natural gas, which requires membrane materials with high permeability, selectivity, and stability of under high pressures. In this work, a high CO 2 -affinity MOF-based nanofiller (P in @NH 2 -UiO-66) was prepared and integrated in polyetherimide (PEI) to prepare mixed matrix membranes (MMMs) for enhanced CO 2 /CH 4 separation capabilities. The P in @NH 2 -UiO-66 nanofiller comprised an in situ-formed polyethyleneimine-NH 2 -UiO-66 composite prepared via a one-pot synthesis. The polyethyleneimine was covalently attached to the H 2 BDC-NH 2 ligand allowing for a stronger integration within the PEI matrix. The polyethyleneimine affects the nucleation of MOF, leading to miniaturization of the MOF particles. The smaller-sized filler is beneficial for improved interaction at the filler-matrix interface. The numerous amino functionalities grafted onto the NH 2 -UiO-66 increased the CO 2 adsorption sites, thereby enhancing the affinity for CO 2 . Owing to the improved interaction, the elevated CO 2 attraction, and the inherent properties of the porous NH 2 -UiO-66, the fabricated MMMs preformed superior in separating CO 2 /CH 4 . The 30-P in @NH 2 -UiO-66-PEI membrane (containing 30 wt% nanofiller) exhibited a CO 2 /CH 4 selectivity of 27.7 and a CO 2 permeability of 2498.9 Barrer. The CO 2 permeability was 21 times greater than that of the pristine PEI membrane, and 4 times higher compared to P@NH 2 -UiO-66 MMM with polyethyleneimine modified MOF filler prepared by a traditional wet impregnation method. Additionally, the novel MMM demonstrates excellent separation stability under conditions that mimic industrial settings, demonstrating its potential application for natural gas purification.

研究领域: 材料科学 · 化学工程
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RSC Advances · 2019 ·Vol. 9 ·期 65 ·37733-37738 · IF 3.049

Temperature modulation of defects in NH2-UiO-66(Zr) for photocatalytic CO2 reduction

Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan

Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.

研究领域: 材料科学 · 环境科学 · 化学工程
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Journal of CO2 Utilization · 2024 · IF 7.2

Structure regulation of two-dimensional lamellar NH2-UIO-66@MXene membrane for efficient H2/CO2 separation

Heming Deng,Haoshuang Gu

Two-dimensional membranes are considered the next generation separation membrane with great application potential due to their excellent separation performance, good mechanical strength and thermal stability compared with traditional membrane materials. In this work, the flexible NH 2 -UIO-66@MXene membrane was successfully prepared for gas separation by loading NH 2 -UIO-66 particles onto Ti 3 C 2 nanosheets based on an in-situ growth strategy. A LiF-HCl mixed solution was used as the etchant to obtain the Ti 3 C 2 nanosheets. The loading of NH 2 -UIO-66 particles can regulate the interlayer spacing of Ti 3 C 2 nanosheets, improving the specific surface area of Ti 3 C 2 and the adsorption capacity for specific gases. The -NH 2 group in NH 2 -UIO-66 enabled preferential adsorption of CO 2 over H 2 , and the CO 2 molecules adsorbed in the channel can even block the molecules passing through, increasing the resistance of CO 2 diffusion. As a result, the NH 2 -UIO-66@Ti 3 C 2 hybrid membrane realizes the selective separation of H 2 /CO 2 mixed gas, and the separation selectivity is as high as 155. The gas separation selectivity and permeation of the final prepared NH 2 -UIO-66@MXene were enhanced and exceeded the upper limit of Robeson upper bound (2017).

研究领域: 材料科学 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Selective photodegradation of tetracycline by molecularly imprinted ZnO@NH2-UiO-66 composites

Qiuzheng Du,Pu Wu,Yiyang Sun,Jingyi Zhang,Hua He

A simple and recyclable imprinted catalytic composite (ZnO@NH 2 -UiO-66, ZUM) was synthesized by postsynthetic modification method with tetracycline (TC) as molecular template. A series of ZUM-n composites with different NH 2 -UiO-66 dopants from 0.1 to 0.7 g had been prepared and compared. The characterization results showed that ZUM-1 possessed the advantages of uniform size, high surface area and wide absorption spectrum. Further research results indicated that ZUM-1 composite has the ability of selective adsorption and the higher photocatalytic degradation efficiency to TC without secondary pollution. Under visible light irradiation, the ZUM-1 could degrade 61.9% of TC within 30 min, which may relate to the inhibition effect of composite materials on electron-hole recombination. The degradation selectivity of ZUM-1 was investigated by comparing the degradation efficiency of TC, tetracycline hydrochloride and ciprofloxacin. The high degradation efficiency and selectivity of ZUM-1 were also confirmed in real samples. The stability experiments showed that the ZUM-1 possessed excellent recyclability and stability in the photocatalytic degradation process, and the recycled process was environmentally friendly. The mechanism of TC photodegradation by ZUM-1 was investigated by UV–vis spectra, photoelectrochemical and radical scavenger experiment. And the possible degradation products were analyzed by HPLC-MS. All in all, this method provided a simple and promising perspective for preparing visible-light-responsive molecular imprinting composites with high specificity and photocatalytic activity.

CAS / MDL: 557-34-6 5970-45-6
研究领域: 环境科学 · 材料科学 · 光催化
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Construction of Bi2MoO6 sheets/NH2-UiO-66(Zr) heterojunction photocatalysts toward enhanced degradation of tetracycline under visible light

Qingqing Wang,Wei Zhou,Claudia Li,Sibudjing Kawi,Yinhui Li

The application of photocatalysts in environmental field has emerged as a prominent research topic. Nevertheless, the efficiency of photocatalysts is reduced as the recombination of photogenerated chargers significantly, restricting their extensive use in this domain. In the present study, photocatalysts composed of bismuth molybdate/NH 2 -UiO-66(Zr) (Bi 2 MoO 6 /NH 2 -UiO-66(Zr)) featuring Z-scheme heterojunctions were effectively synthesized using a two-step hydrothermal technique. These photocatalysts exhibit remarkable photocatalytic degradation under visible light conditions. Notably, the broad planar configuration of Bi 2 MoO 6 sheets improves the separation of the photogenerated charge carriers. NH 2 -UiO-66(Zr) layered atop Bi 2 MoO 6 sheets enhances the availability of catalytically active sites, reduces charge recombination, and promotes charge transfer through the interface. The kinetic rate constant for Bi 2 MoO 6 /NH 2 -UiO-66(Zr) is around 0.00329 L mg −1 min −1 , indicating the increase of 3.78 and 41.13 times compared with pure Bi 2 MoO 6 and NH 2 -UiO-66(Zr), respectively. The efficiency for photocatalytic degradation of tetracycline using Bi 2 MoO 6 /NH 2 -UiO-66(Zr) reaches 81.72 % under visible light. Importantly, this efficiency exhibits a reduction of 10 % after five recycling cycles, demonstrating notable stability. The photocatalytic mechanism involved in tetracycline degradation was uncovered through trapping experiments and EPR, indicating that it is predominantly facilitated by the active oxidation of ·O 2 - and ·OH. The intermediates of the photocatalytic process as well as the possible degradation pathways were discussed. The creation of Bi 2 MoO 6 sheets/NH 2 -UiO-66(Zr) heterojunction photocatalysts provides a fresh approach to the development of novel catalysts, which may lead to significant advancements in environmental remediation efforts.

研究领域: 环境科学 · 材料科学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

NH2-UiO-66 Coated with Two-Dimensional Covalent Organic Frameworks: High Stability and Photocatalytic Activity

Yongchao Wang,Qing Yang,Fangli Yi,Ruowei Lu,Yanxia Chen,Cheng Liu,Xinyu Li,Cuijuan Wang,Hongjian Yan

The poor stability and low catalytic activity of NH2-UiO-66 in basic solutions require the reactions to be conducted in acidic solutions, which seriously hinders its potential photocatalytic application. Herein, we report that NH2-UiO-66 coated with two-dimensional covalent organic frameworks (COFs) via imine bond connection presents not only high photocatalytic activity but also high stability and adaptability to the solution environment. The NH2-UiO-66/COF hybrid material was fabricated through the Schiff base reaction of NH2-UiO-66 with 4,4′,4″-(1,3,5-triazine-2,4,6-triyl)trianiline (TAPT) and 2,4,6-triformylphloroglucinol (TP). The hybrid material showed high stability in an alkaline environment, with only 4.7% of NH2-UiO-66 decomposed after the photocatalytic reaction. The optimum photocatalytic H2 evolution rate was 8.44 mmol·h–1·g–1 when triethanolamine was used as an electron-donating agent. The results presented here illustrate the possibility for effectively improving both the photocatalytic performance and stability of NH2-UiO-66 by coupling with COFs.

研究领域: 材料科学 · 光催化领域
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Immobilization of Nickel- and Cobalt-Based Complexes in NH2-UiO-66 for Efficient CO2 Photoreduction

Yu Jiang,Si-Chao Liu,Li-Ping Zhang,Guo-Wei Guan,Yi-Tao Li,Shuang Ni,Run-Yuan Jiang,Su-Tao Zheng,Hao-Ran Liu,Hao-Ling Lan,Qing-Yuan Yang

The photocatalytic reduction of carbon dioxide (CO 2 ) to carbon-based materials is challenging because of its intricate nature and the generation of multiple byproducts. Hence, developing photocatalysts with a high CO 2 -reduction yield and selectivity is critical. In this study, new photocatalysts (U-B-M, M = Co, Ni) were synthesized by incorporating 1,2-benzisothiazolin-3-one (BIT) into NH 2 -UiO-66, to create N, N’-chelating sites via an amine–aldehyde condensation reaction, followed by metal-ion chelation. The introduction of BIT decreased the resistance of the catalyst and enhanced the separation of photogenerated carriers. The catalytic performance of U-B-Ni (rate: 3.10 mmol·g −1 ·h −1 ; selectivity: 97 %) surpasses those most of all previously reported MOF-based photocatalysts. Moreover, U-B-Ni shows high stability and negligible deactivation on catalytic cycling for over 16 h. This study expands the utility of metal–organic frameworks (MOF) in photocatalysis and highlights the importance of amine–aldehyde condensation in MOF modification.

研究领域: 材料科学 · 环境科学 · 化学工程
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MICROCHIMICA ACTA · 2021 ·Vol. 188 ·期 2 ·1-11 · IF 5.833

Determination of acetamiprid using electrochemiluminescent aptasensor modified by MoS2QDs-PATP/PTCA and NH2-UiO-66

Li Jingxian,Jiang Ding,Shan Xueling,Wang Wenchang,Ou Guofu,Jin Haozhe,Chen Zhidong

A novel aptasensor has been fabricated based on the resonance energy transform (RET) system from MoS 2 QDs-PATP/PTCA (donor) to NH 2 -UiO-66 (acceptor). The electrochemiluminescence (ECL) signal of PTCA was greatly amplified due to the decoration of MoS 2 QDs-PATP, and the NH 2 -UiO-66 was utilized to label the signal probe DNA (pDNA), which hybridizes with the exposed aptamer anchored on the surface of MoS 2 QDs-PATP/PTCA. With the target acetamiprid, the specific binding of acetamiprid to aptamer causes the connection between the donor and the acceptor to be interrupted and produce an “on” ECL signal. Thus, an “off-on” ECL sensing platform for sensitive and selective acetamiprid assay was designed. Under the optimal condition, the ECL signal of the aptasensor was found to be linearly related to the logarithm of the acetamiprid concentration ranging from 0.1 fM to 0.1 μM with a detection limit of 0.064 fM. More importantly, the recovery rate of the ECL aptasensor was calculated to be 98.7 ~ 106% with a RSD lower 5.1% for the residual acetamiprid assay in real food samples, which indicated that the aptasensor has high potential for practical applications. Graphical abstract

研究领域: 分析化学 · 环境科学 · 食品科学
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RSC Advances · 2020 ·Vol. 10 ·期 3 ·1757-1768 · IF 3.119

A direct Z-scheme Bi2WO6/NH2-UiO-66 nanocomposite as an efficient visible-light-driven photocatalyst for NO removal

Yiqiu Liu,Yi Zhou,Qijun Tang,Qian Li,Si Chen,Zhuxing Sun,Haiqiang Wang

To explore an efficient photocatalyst for NO pollution, a direct Z-scheme photocatalytic system is successfully fabricated by coupling Bi2WO6 with NH2-UiO-66 via a simple hydrothermal synthesis technique. The Z-scheme system promotes the NO photocatalytic oxidation activity with an optimum NO removal rate of 79%, which is 2.7 and 1.2 times that obtained by using only pristine Bi2WO6 and NH2-UiO-66, respectively. Simultaneously, superior selectivity for converting NO to NO3−/NO2− is observed. The enhanced photocatalytic performance of the Bi2WO6/NH2-UiO-66 hybrids is attributed to the following two aspects: (i) large specific area of NH2-UiO-66, which exposes more active sites and is beneficial to the adsorption and activation of NO; (ii) outstanding Z-scheme structure constructed between BiWO6 and NH2-UiO-66, which can improve the efficiency of the separation of electron–hole pairs and preserves the strong oxidation ability of hybrids. ESR analysis shows that ·O2− and ·OH contribute to NO removal. A possible photocatalytic mechanism of NO oxidation on the direct Z-scheme photocatalyst (BWO/2NU) under visible light irradiation is proposed. This work displays the BWO/2NU hybrid's potential for treating low-concentration air pollutants, and the proposed Z-scheme photocatalyst design and promotion mechanism may inspire more rational synthesis of highly efficient photocatalysts for NO removal.

CAS / MDL: 10035-06-0 10213-10-2
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Three-Dimensional g-C3N4/NH2-UiO-66 graphitic aerogel hybrids with recyclable property for enhanced photocatalytic elimination of nitric oxide

Zhou Zhou,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu

In order to fix the photocatalyst and enhance the efficiency of NO degradation, a three-dimensional (3D) g-C 3 N 4 /NH 2 -UiO-66-rGO (CN/NU6-rGO) aerogel was devised and fabricated via solvothermal reaction and boiling-water bath. Herein, a type-II heterojunction was formed at CN/NU6 composite, and then, the composite was coupled with rGO. The resulting material significantly enhanced the nitric oxide (NO, 600 ppb) removal efficiency under visible-light irradiation. Optimizing the content of CN and rGO to a suitable mass ratio can increase the removal efficiency by 65.4%, which is 2.34 times that of pure NU6. This result is attributed to the construction of type-II heterojunction and the charge transport properties of rGO. The involvement of rGO not only provided extra pathways for charge transfer to prevent electron–hole pairs from recombining, but also fixed the catalyst. Moreover, the hybrid aerogel excellently reduced the harmful by-product NO 2 . Cycling experiments, along with transient photocurrent response measurements, verified that CN/NU6-rGO had excellent potential for recyclable and sustainable. This work might shed light on the construction of suitable photocatalytic systems with significant improvement of NO removal and convenient storage of catalyst.

CAS / MDL: 10026-11-6
研究领域: 材料科学 · 环境科学 · 化学
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Co-doped NH2-UiO-66 for fast and effective adsorption of oxytetracycline: Kinetics, thermodynamics and mechanism

Yi Wang,Tao He,Siying Lv,Jing Yang,Shihai Cui

Novel type of micro mesoporous materials Co-doped NH 2 -UiO-66 had been successfully prepared. The properties of the material were understood through a series of characterization. When the dosage of Zr:Co is 2:1, the modified material showed specific surface area of 840.02 m 2 ∙g −1 , which is larger than the material without Co. Especially, the material was transformed from microporous NH 2 -UiO-66 to micro-mesoporous Co-doped NH 2 -UiO-66 through the adjustment of metal Co. The Co-doped nanocomposite was then applied to the adsorption of oxytetracycline. The effects of initial concentration, pH, humic acid and ionic strength on the adsorption were investigated. It was found that 50 mg∙L −1 oxytetracycline can be effectively adsorbed by Co-doped NH 2 -UiO-66 in pH 7. Further research showed that adsorption was pseudo-second-order kinetics and fitted Freundlich model with the maximum adsorption capacity 223.7 mg∙g −1 . In addition, the adsorption equilibrium time was only 2 h, which is shorter than the adsorption time of most adsorbents. The mechanism of pore adsorption, π-π interaction, hydrogen bonds and electrostatic interactions was deeply discussed. In conclusion, Co-doped NH 2 -UiO-66 was a fast and effective absorbent for the removal of oxytetracycline in aqueous solution.

研究领域: 环境科学 · 材料科学
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