ANALYST
·
2023
·
IF 4.2
Rongqiu Yan,Qiongfang Zhou,Hui Xie,Chenghong Lei
Au nanoparticle-embellished metal-organic frameworks UiO-66 on reduced graphene oxide (Au/UiO-66/rGO) was synthesized. Au/UiO-66/rGO displayed strong electrocatalytic activity for oxidation of glucose in alkaline solution at a remarkable low oxidation potential at +0.20 V vs. Ag/AgCl. Au nanoparticles played a paramount role for catalytic oxidation of glucose at the electrode, while both rGO and UiO-66 can significantly enhance the current responses to glucose. The resulting non-enzymatic glucose sensor exhibited a wide range of linear response, high sensitivity and selectivity for the determination of glucose. The sensor was successfully applied for the determination of glucose in honey product.
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PubMed
高影响因子
Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yaping Wu,Xingyue Hong,Zhenying Li,Yanting Lei,Rongfei Yu,Taoli Deng,Yutao Zhang,Peihua Ma
Different ligand functionalized bimetallic organic framework ((Zr/Ce)UiO-66- X ( X = H, NO 2 , NH 2 and (OH) 2 ) solids-supported phosphotungstic acid (HPW) has been fabricated through a facile impregnation process, and used in the esterification of methanol with oleic acid (OA). The obtained composites were characterized by FTIR , XRD, NH 3 -TPD, SEM-EDS, N 2 adsorption-desorption isotherm, TG , Py-FTIR, and XPS. The characterization analysis shows that the HPW/(Zr/Ce)UiO-66-NO 2 composite possesses the proper catalytic features, such as the greatest number of both strong Brønsted and Lewis acid sites, wider pores, relatively high surface area, and the existence of synergistic catalytic effects between HPW and (Zr/Ce)UiO-66-NO 2 framework. In the screening, the maximum OA conversion rate using (Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66, HPW/(Zr/Ce)UiO-66-NH 2 , HPW/(Zr/Ce)UiO-66-(OH) 2 catalysts is 13.7%, 91.6%, 81.6%, 80.7%, and 72.6% at 110 °C for 3 h, respectively. Moreover, the HPW/(Zr/Ce)UiO-66-NO 2 catalyst presents the better reusability over four cycles. Besides these, the HPW/(Zr/Ce)UiO-66-NO 2 catalyzed esterification reaction is estimated to have an activation energy of 33.7 kJ/mol. This present study provides an effective route for realizing biofuel production on an industrial scale involving heteropolyacids/bimetallic MOFs synergistic catalysts.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Chong Chen,Xue Li,Weixin Zou,Hui Wan,Lin Dong,Guofeng Guan
Methane is regarded as a potential alternative energy and chemical raw material, and its separation from biogas by capturing CO 2 has become a hot issue of great significance and challenge. Taking the low partial pressure of CO 2 in biogas (~50% CO 2 and ~50% CH 4 ) into consideration, a facile pre-synthetic method was applied to endow UiO-66-NH 2 with high adsorption capacity and selectivity toward CO 2 , via interligands cross-linking of two-molecule 2-aminoterephthalic acids through amidation reaction. At 298 K, the CO 2 uptakes of UiO-66-DAM at 0.5 and 1 bar were 36.7 and 54.1 cm 3 ·g −1 respectively, which were 16.9% and 12.7% higher than those of UiO-66-NH 2 . Meanwhile, the CO 2 /CH 4 selectivity of UiO-66-DAM at 1 bar was 1.43 times that of unlinked framework. It could be speculatively attributed to the cooperative effects of amide functional groups and smaller pore diameter of UiO-66-DAM, which synergized with open Zr(IV) sites to enhance the binding affinity toward CO 2 . Moreover, the higher isosteric heats of adsorption for modified MOF at low loading also revealed the strong interactions between polar pore surfaces and guest CO 2 molecules. Along with the highly reversible adsorption-desorption behavior during recycling, the ligand-cross-linked UiO-66-DAM could be very promising for future practical applications of selective gas separation.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14868-14876
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IF 12.732
Liangjie Wang,Juan Li,Luyao Cheng,Yonghui Song,Ping Zeng,Xianghua Wen
Metal organic frameworks (MOFs), emerging adsorbents and catalysts in the wastewater treatment field, are subject to destruction by Lewis bases in wastewater, such as F− and PO43−. To promote the application of MOFs in wastewater treatment, it is imperative to clarify the mechanism of the destructiveness of L-bases to MOFs. Accordingly, in this study, we performed a series of deliberately designed experiments and theoretical analyses. The ligand release of MOFs in solutions of various L-bases indicated that the order of destructiveness of L-bases to UiO-66-type MOFs was OH− > F− > PO43− > AsO43− > SO42− > CO32− = Ac− = Cl− = Br− = NO3− = 0. To elaborate the intrinsic nature of the destructiveness of L-bases to MOFs based on hard and soft acid base theory, density functional theory was used to calculate the various physicochemical parameters of L-bases related to their strength, including chemical potential (μ), Mulliken electronegativity (χ = −μ), chemical hardness (η), local softness for electrophilic attack (s−) and charges of coordinating atoms (CCA). Among these parameters, μ (−χ) and CCA can reflect the destructiveness of L-bases to MOFs to a large extent, with higher μ (−χ) and CCA indicating higher destructiveness. To more accurately judge the destructiveness of L-bases to MOFs, integrated use of both μ (−χ) and CCA is suggested. Additionally, the stability of some UiO-66-type MOFs cannot be well judged by μ (−χ) and CCA due to the deformation of their ligand structure caused by the steric hindrance of the functional groups of the ligand.
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MICROCHEMICAL JOURNAL
·
2019
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IF 3.206
Yajun Zhang,Xiaoliang Zeng,Xiaofang Jiang,Hanjiao Chen,Zhou Long
The cerium (Ce)-based UiO-66 metal-organic frameworks were employed for the first time as an effective catalyst for both oxidation and reduction. On one hand, selenium (Se)(VI) was efficiently photo-reduced to volatile species derived from the low lying of Ce 4f orbital and efficient generation of photo-electrons through the frameworks of UiO-66(Ce); on the other hand, the chromogenic substrate, 3, 3′, 5, 5′-tetramethylbenzydine (TMB), was oxidized based on the oxidase-like behavior of UiO-66(Ce) derived from the Ce 4+ /Ce 3+ spontaneous redox couple. The photo-reduced Se(VI) was determined by atomic fluorescence spectrometry , with a linear range of 5.0–200.0 μg/L − 1 , correlation coefficient of 0.998, and detection limit of 1.5 ng/mL − 1 obtained. The colorimetric sensing of mercury (Hg)(II) was accomplished based on the inhibition of TMB oxidation via Hg (II)-TMB interaction, with two linear ranges of 0.1–2.0 μM and 2.25–4.1 μM obtained, and a correlation coefficient of 0.993 and 0.995 obtained, respectively. The catalytic activity of UiO-66(Ce) was demonstrated to be satisfactory for both oxidation and reduction, which further explored the application of UiO-66(Ce) in the field of catalysis.
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Catalysis Science & Technology
·
2015
·Vol. 6
·期 3
·869-874
·
IF 5.426
Shu-Tao Gao,Weihua Liu,Cheng Feng,Ning-Zhao Shang,Chun Wang
Highly dispersed Ag–Pd alloys deposited on an amine-functionalized UiO-66(NH2–UiO-66) have been successfully prepared via a pre-coordination method. The as-synthesized AgPd@NH2–UiO-66 catalyst exhibited 100% H2 selectivity and a high catalytic activity (TOF = 103 h−1) toward the dehydrogenation of formic acid at room temperature without any additives, which is among the highest values ever reported. Our study further reveals that the synergetic effect between the Ag–Pd alloy and NH2–UiO-66 support play a key role for the efficient catalytic dehydrogenation of formic acid.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Yongfeng Liu,Lijuan Ding,Ang Yan,Jianteng Wei,Yi Liu,Yuzhong Niu,Rongjun Qu
To achieve simultaneous adsorption removal of anionic and cationic dyes, UiO-66-NH 2 @Dodecyl functionalized with dodecyl (long-chain alkane) and UiO-66-NH 2 @PEI modified by polyethyleneimine (PEI) (containing multiple amino groups) were facilely fabricated by post-synthesis functionalization strategy, and characterized systematically. UiO-66-NH 2 @Dodecyl and UiO-66-NH 2 @PEI both showed higher adsorption capacities for Congo red (458.2 and 583.4 mg/g) and methylene blue (218.0 and 286.3 mg/g). Adsorption kinetic and isotherm curves could be simulated best by pseudo-second-order kinetic model and Langmuir isotherm model, respectively. Under coexistence of inorganic salts and alkalinity, it was beneficial to improve adsorption capacities. Adsorption capacity of UiO-66-NH 2 @PEI with multiple amino groups was higher than UiO-66-NH 2 @Dodecyl at the same experimental conditions, indicating that hydrogen bonding had greater influence on adsorption efficiency. And UiO-66-NH 2 @Dodecyl and UiO-66-NH 2 @PEI had better stability. Hydrogen bonding, π-π conjugation, electrostatic interaction and van der Waals force were main adsorption driving forces. The results could provide theoretical and technical help for simultaneous adsorption removal of anionic and cationic dyes.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhizhou Liu,Le Ma,Xueyan Nan,Xiang Zhao,Liang He,Tong Wang,Pengli Bai
Non-specific binding was a critical bottleneck in biosensing field and hindered the implementation of biosensors in bioassays. Thus, various approaches were developed to minimize the non-specific binding of biosensors. However, the rational utilization of non-specific binding will also produce generous returns. Herein, the first universal cell surface barcoding strategy for mass cytometry independent on particular cell surface molecules was developed based on nano-sized UIO-66 typed metal organic framework (MOF). Profiting from the 9 abundant stable isotopes of Zr and Hf, up to 84 mass barcode combinations can be achieved theoretically through the non-specific binding between positively charged UIO-66 and negatively charged cells. Clearly distinguished individual population sets were obtained when the cell samples were barcoded with UIO-66(Zr), UIO-66(Hf), and UIO-66(Zr/Hf) mixture. UIO-66 can also be used for flow cytometry barcoding and imaging after the modification with a fluorescent dye. Furthermore, the UIO-66 barcoding showed high compatibility with metal chelated polymer (MCP) mass tags in single-cell multiplexing and 16-fold higher sensitivity than MCP based barcoding agents. This work opens new opportunities for MOFs in mass cytometry applications and will also prompt people to evaluate the nasty non-specific binding in another perspective.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Ying Zhang,Tianya Cao,Baoqing Bai,Xu Jing,Ligang Yu,Jinhua Zhang,Tao Bo,Huilin Liu,Ying Gu,Yukun Yang
The hazard of diethylstilbestrol (DES) towards human health underscored the imperative for highly sensitive and rapid analytical technologies. Herein, a molecularly imprinted electrochemical sensor (MIECS) was innovatively constructed by incorporating the Pt nanoparticles (PtNPs)-decorated MXene/NH 2 -UiO-66 into molecularly imprinted polymer (MIP/MXene/NH 2 -UiO-66/PtNPs) for ultra-sensitive and rapid detection of DES. The introduction of NH 2 -UiO-66 effectively prevented the restacking of MXene and with the synergistic effect of PtNPs, the electrical conductivity of the sensor was significantly enhanced. MIP/MXene/NH 2 -UiO-66/PtNPs-based MIECS not only exhibited excellent electrical conductivity but also possessed the specific cavity to recognize DES. Under optimal experimental conditions, the MIP/MXene/NH 2 -UiO-66/PtNPs-based MIECS exhibited a good relationship with the concentration of DES over a wide range of 1 × 10 −11 –1 × 10 −4 mol L −1 and an extremely low detection limit (1.19 × 10 −12 mol L −1 ). This study demonstrates the judicious design of ternary composite via hetero-interface engineering in the construction of MIECS, providing a new idea for electrochemical sensing.
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PubMed
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yiyang Liu,Hengyuan Zhang,Dechang Xie,Huiyu Lai,Qiufeng Qiu,Xiaoguo Ma
Macrolide antibiotics (MALs) are widely used in various fields and are resistant to degrade in the water environment, thus constituting potential hazards to human health. In this work, a new composite, molecularly imprinted polymers coated magnetic metal-organic frameworks with carboxyl modification ( [email protected] ) was selected and characterized, for the simultaneous specific adsorption and determination of five MALs from aqueous solution. It was found that UIO-66-COOH with ligand defects showed better pre-polymerization effect than other matrix materials . The synthesis conditions for the imprinting polymer were optimized via response surface methodology . The characteristics of related materials were studied, and a series of adsorption experiments were carried out. The results showed that the adsorption equilibriums of [email protected] were reached within 1 h, with the total adsorption capacity for the five MALs was 99.05 mg g −1 . The pseudo-second-order kinetic model and Freundlich isotherm model could best fit the adsorption process , and the adsorption thermodynamics was controlled by the change of entropy. Adsorption mechanisms were deduced as hydrogen bonding interaction and electrostatic interaction. In addition, [email protected] has good selectivity and reusability. Furthermore, a new detection method for the five MALs was developed, using the prepared material as the adsorbent for magnetic solid-phase extraction, coupled with high-performance liquid chromatography . Under the optimal extraction condition, the limits of detection for five MALs were 3.1–44.6 μg L −1 , and the recoveries were 92.9–108.7 % in the determination of real water samples. Therefore, the [email protected] could be the efficient adsorbent for simultaneous selective removal and sensitive determination of multi-residual MALs.
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ANALYST
·
2020
·Vol. 145
·期 9
·3245-3256
·
IF 3.978
Liping Xu,Jiebin Li,Jiajia Zhang,Junyong Sun,Tian Gan,Yanming Liu
In this work, a disposable molecularly imprinted electrochemical sensor was developed towards the highly sensitive and selective detection of the organophosphorus insecticide phosalone (PAS), employing a home-made carbon paste microelectrode (CPME) modified with a Zr-based metal–organic framework catalyst (Pt-UiO-66) and a mesoporous structured conductive molecularly imprinted polymer (MIP). Pt-UiO-66 octahedra with isolated dispersed Pt nanoparticle active sites were firstly incorporated into the CPME to provide a remarkably amplified signal for voltammetric determination. The mesoporous MIP was then synthesized onto the Pt-UiO-66/CPME via electropolymerization and a subsequent sol–gel process, which could bind the PAS template molecules through hydrogen bond, coordinate bonding, hydrophobic interaction, and π–π stacking interaction. Morphological, structural, and electrochemical characterization studies revealed that this nano-sized MIP provided excellent features for PAS detection, including high porosity, large surface area, enhanced electron-transport ability, greatly improved diffusion capacity, and strong recognition specificity. Therefore, the resulting sensor exhibited an outstanding linearly proportional concentration domain of 0.50 nM–20 μM, low detection limit of 0.078 nM, marked selectivity over certain interferences with similar configurations, considerable repeatability, reproducibility, and stability for the analysis of PAS. Moreover, the sensor was successfully applied for the determination of PAS in agricultural products and environmental samples with results in good compatibility with a chromatographic method, indicative of the high reliability and practicability. Such an electrochemical sensor might open a novel window for the investigation of selective sensing of small organic species from their analogues coupled with the molecular imprinting technique.
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PubMed
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Xiaoyu Bai,Peng Liu,Xingtong Gao,Kai Liu,Aixiang Li,Zijian Lyu,Qiuhong Li
It is a major obstacle to further development of membrane technology that membrane fouling occurs. In this study, a novel Fe 3 O 4 @UiO-66-NH 2 /PVDF-co-CTFE mixed matrix membrane was successfully developed by mixing Fe 3 O 4 @UiO-66-NH 2 nanoparticles (NPs) into PVDF-co-CTFE membrane through a simple non-solvent-induced phase separation (NIPS) method, and was used for degradation of organic wastewater. The results of the incorporated Fe 3 O 4 @UiO-66-NH 2 NPs content on the morphology, pore structure and physicochemical structure of samples were investigated systematically. The results indicated that the Fe 3 O 4 @UiO-66-NH 2 NPs addition in membrane matrix improved the permeability and significantly enhanced the anti-fouling performance. When 2 wt% Fe 3 O 4 @UiO-66-NH 2 NPs was added, the mixed matrix membrane had excellent comprehensive performance, maintaining a high pure water flux of 226.8 L m −2 h −1 , the BSA rejection rate reached 95.9%, and the flux recovery rate was 71.38%. Importantly, the membrane possessed high catalytic performance based on the Fenton reaction mechanism, and the removal rate of 20 mg L −1 MB solution (400 mL) was up to 99.04%, and showed excellent self-cleaning characteristics and long-term stability. In conclusion, this study provided a new idea for the development of Fenton catalytic membranes with excellent anti-fouling performance for wastewater treatment in complex environments.
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