ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 2
·1-11
·
IF 5.3
Sun Xueqin,Fan Yan,Zhang Wenyuan,Yang Xiaogang,Liu Jiacheng
A pentafluoropropionic acid–functionalized fluorescent metal–organic framework material (UiO-66-NH 2 -PFPA) is prepared by a simple post-synthetic modification (PSM) strategy for the sensitive and selective detection of dichloran (DCN). The results of fluorescence experiments demonstrate that the sensitivity of UiO-66-NH 2 -PFPA (limit of detection, LOD = 0.478 μM) to DCN is nearly 10.93 times higher than that of UiO-66-NH 2 (LOD = 5.225 μM) and the material has good selectivity and anti-interference ability. After the addition of DCN, the blue fluorescence of UiO-66-NH 2 -PFPA is obviously quenched. Therefore, the possible quenching mechanism is further discussed in combination with relevant experiments and density functional theory calculations. Moreover, the sensor is applied to the detection of DCN in fruit samples with a satisfactory recovery of 101.1—107.9%, which implies that UiO-66-NH 2 -PFPA is expected to be a candidate material for the detection of DCN in food. Graphical abstract
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Li Gong,Yijiao Zhang,Renlong Liu,Zuohua Liu,Siwei Jin,Li Zhang,Tengda Zhao,Huanbao Fa,Wei Yin
Due to the toxicity and corrosiveness of the ammonia gas, low-cost, portable, and accurate methods of ammonia detection are of great importance in environmental testing and disease diagnosis. In this study, flower-like UIO-66-NH 2 @MoS 2 composite modified screen-printed electrodes (SPEs) were prepared by hydrothermal treatment using ionic liquids [BMIM][BF 4 ] as electrolytes. The UIO-66-NH 2 @MoS 2 /SPEs were then combined with a miniature electrochemical workstation to construct a novel electrochemical ammonia sensor. The experimental results showed that UIO-66-NH 2 @MoS 2 had excellent adsorption capacity for ammonia, exhibiting good linearity in the range of 5–500 ppm with a low limit of detection (2.1 ppm) and a fast response time for 100 ppm ammonia (13 s). This sensor also possessed excellent stability, reproducibility, and anti-interference ability. The synthesized UIO-66-NH 2 @MoS 2 nanocomposite was demonstrated to be an excellent candidate for the construction of high-performance ammonia sensors for various applications.
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TALANTA
·
2024
·
IF 5.6
Kexin Xu,Jinhui Zhu,Tong Zhang,Guodong Sui
Wastewater-based epidemiology (WBE) is a powerful tool for early warning of infectious disease outbreaks. Hence, a rapid and portable pathogen monitoring system is urgent needed for on-site detection. In this work, we first reported synthesis of an artificial modulated wide-spectrum bacteria capture nanoparticle (Arg-CSP@UiO@Fe 3 O 4 ). Arginine-modified phosphorylated chitosan (Arg-CSP) coating could provide strongly positive charged guanidinium group for pathogen interaction by electrostatic attraction, and UiO-66-NH 2 layer could help Arg-CSP graft onto Fe 3 O 4 magnetic particles. The capture efficiency of Arg-CSP@UiO@Fe 3 O 4 reached 92.2 % and 97.3 % for Escherichia coli ( E.coli ) and Staphylococcus epidermidis ( S.epidermidis )within 40 min, in 10 mL sample. To prevent pathogen degradation in sewage, a portable nucleic acid extraction-free method was also developed. UiO-66-NH 2 could disintegrate in buffer with high concentration of PO 4 3− for bacterium desorption, and then nucleic acid of the bacteria was released by heating. The DNA template concentration obtained by this method was 779.28 times higher than that of the direct thermal lysis product and 8.63 times higher than that of the commercial kit. Afterwards, multiple detection of bacteria was realized by loop-mediated isothermal amplification (LAMP). Artificial regulated pathogen desorption could prevent non-specific adsorption of nucleic acid by nanoparticles. The detection limit of Arg-CSP@UiO@Fe 3 O 4 -LAMP method was 80 cfu/mL for E.coli and 300 cfu/mL for S.epidermidis . The accuracy and reliability of the method was validated by spiked sewage samples. In conclusion, this bio-monitoring system was able to detect multiple bacteria in environment conveniently and have good potential to become an alternative solution for rapid on-site pathogen detection.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
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IF 8.3
Ruyi Cui,Yong Zhou,Xingyi Xu,Hengxin Fang,Wenlong Wang,Sanmei Wang,Pengbo Lyu,Lizhong Sun,Biao Wang,Changqing Sun
Ammonia borane (AB) is a highly promising hydrogen carrier with significant potential for safe and efficient hydrogen storage and transportation. However, its high chemical stability poses considerable challenges for hydrogen release, emphasizing the importance of highly efficient catalysts. In this study, we present Ru nanocatalysts supported on UiO-66-NH 2 -derived carbon nitride (Ru/CN) as high-performance catalysts for AB hydrolysis. A facile pyrolysis-impregnation method was employed to synthesize highly dispersed Ru nanoparticles with tunable sizes, while retaining the octahedral morphology of the MOF-derived support. Detailed characterizations revealed tunable Ru nanoparticle sizes achieved by simply adjusting the Ru loading. Among the catalysts, the 2.5Ru/CN, featuring Ru nanoparticles with an average size of 2.2 nm, achieved an impressive turnover frequency of 493 mol H 2 (mol Ru −1 ·min −1 ) at 30 °C, demonstrating exceptional catalytic activity. Density functional theory (DFT) calculations confirmed that the optimized Ru cluster size enhances key catalytic steps, including H 2 O dissociation, AB activation, and H 2 desorption. This study highlights the critical role of fine-tuning nanoparticle sizes and provides valuable insights into the rational design of advanced catalysts for more efficient hydrogen production.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Xiaoyu Du,Gan Wu,Xilin Dou,Zhaoyang Ding,Jing Xie
Food prone to spoilage has a huge food safety hazard, threatening people’s health, so early detection of food spoilage is a continuous and urgent need. Herein, we developed a dual-mode response sensor, alizarin complexone@UiO-66-NH 2 , which can accurately detect pH. The sensor demonstrated significant changes in color from pale yellow to deep pink, while the fluorescence shifted from light blue to blue violet. Moreover, both UV absorption and fluorescence intensity showed a linear correlation with pH raging from 4.5 to 7.5. These results indicate that the sensor effectively responds to pH, making it suitable for detecting the freshness of perishable food. To put this into practice, we integrated the sensor with cellulose-based filter paper to determine the freshness of shrimp and beef, which was proved to be effective in assessing freshness. In the future, it can be combined with intelligent colorimetric and fluorescence instruments to achieve visual detection.
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Analytical Methods
·
2020
·Vol. 12
·期 41
·4967-4976
·
IF 2.596
Xin Yao,Jinhui Shen,Qingyan Liu,Huanbao Fa,Mei Yang,Changjun Hou
In this work, we designed and synthesized a nanocomposite comprising an amine-functionalized metal organic framework (UiO-66-NH2), a multiwalled carbon nanotube@reduced graphene oxide nanoribbon (MWCNT@rGONR) and a covalent organic framework (COF) synthesized using melamine and cyanuric acidmonomers via polycondensation (represented by MCA). The UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite was used as a sensitive platform for an electrochemical aptasensor to detect kanamycin (kana). Owing to the rich chemical functionality, amino-rich structure and excellent electrochemical activity, the cDNA strands with terminal amino groups can not only anchor over the UiO-66-NH2/MCA/MWCNT@rGONR surface but also penetrate into the interior of porous UiO-66-NH2/MCA/MWCNT@rGONR networks. The characterization of the UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite was performed by scanning electronic microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectroscopy and X-ray diffraction (XRD). Furthermore, cyclic voltammetry (CV) and square wave voltammetry (SWV) were employed for the electrochemical performance study of this biosensor. The results indicated that the UiO-66-NH2/MCA/MWCNT@rGONR nanocomposite exhibited high bioaffinity toward the aptamer and the lowest limit of detection at 13 nM (S/N = 3) within a linearity of the kana concentration of 25–900 nM. In addition, it possessed great repeatability, stability and selectivity and obtained satisfactory recovery results in the real analysis of fish meat and milk, indicating the great potential for analytical measurements in food safety.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Lingtao Liu,Lijian Wang,Jingxin Tan,Cong Yu,Junjie Bian,Xinbo Wang
Photocatalytic selective oxidation of furfural is a green, gentle way of preparing furoic acid. Photocatalytic oxidation effectively avoids the problems of difficult separation and high energy consumption in subsequent work-ups caused by the use of homogeneous oxidants. The photocatalytic process suffers from uncontrollable reactive oxygen species, resulting in low selectivity of the target product and excessive oxidation. Therefore, the K x -C 3 N 4 /UiO-66-NH 2 -Y catalyst was prepared by the mass proportion of UiO-66-NH 2 and K x -C 3 N 4 to form a heterogeneous structure, and the band gap width was adjusted to effectively avoid the formation of non-target strong reactive oxygen species ( OH). The results showed that: the aqueous 0.1 mM Na 2 CO 3 solution had an inhibitory effect on the non– target reactive oxygen species at room temperature; when the reaction time was 5 h and K 0.1 -C 3 N 4 /UiO-66-NH 2 -20, the furoic acid had the highest yield of 70.7, the target reactive oxygen species was confirmed by free radical capture experiments as O 2 – , and it was postulated that the reaction mechanism for the preparation of furoic acid by selective oxidation of furfural.
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Water Conservation Science and Engineering
·
2025
·Vol. 10
·期 3
·1-16
·
IF 1.9
Li Zhengjie,Fang Chunxia,Ma Xilong,Liu Yixian,Xie Juan,Li Pengfei,Zhang Zhikun,Zhao Xudong,Sun Hua,Han Jilong
Herein, a facile and rapid preparation method was developed to synthesize Ce-doped UiO-66-NH 2 through a one-pot solvothermal method. This approach simultaneously introduces functional groups onto organic ligands and incorporating a novel metal into metal clusters. The incorporation of Ce ions effectively enlarged the pore size and increased the pore volume, thereby facilitating the diffusion of specific adsorbate molecules into the inner adsorption sites provided by the –NH 2 groups. Due to the favorable pore structures and more exposed adsorption sites, the safranine T (ST) adsorption capacity of Ce-doped UiO-66-NH 2 was ten times higher than the pristine UiO-66-NH 2 and reached 1340 mg/g at optimal adsorption conditions, surpassing most of the reported porous adsorbents. The kinetic and isotherm fitting results showed that the pseudo-second-order and Langmuir models described the adsorption behaviors of ST best, indicating a homogeneous, endothermic, and spontaneous monolayer adsorption process. The adsorption mechanism showed that the hydrogen bonding interaction and pore filling effect are identified as the main mechanism whilst electrostatic attraction interaction further enhances the adsorption capacity at optimal pH. Therefore, Ce-doped UiO-66-NH 2 can serve as a promising adsorbent for the removal of cationic dyes from textile wastewater, and the developed facile and rapid method offers a viable strategy to construct novel MOF-based adsorbents.
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Fujian Xu,Jinyi Zhang,Xiaoliang Zeng,Zhou Long,Xiandeng Hou
Alkaline phosphatase (ALP) is now a well acknowledged indicator for diverse clinical diseases correlated with its abnormal expression. Compared to the assays by traditional and lately emerging methods, the fluorescent (FL) sensing, especially in the turn-on mode, has become more favored due to its simplicity, low cost, and high sensitivity and precision. However, the feasible FL probes are still limited and suffering from poor biological compatibility, complex preparation, additional modification or function-alization. Herein, we found that one common metal–organic framework, UiO-66-NH 2 at nanoscale, could act as a new and label-free FL probe for facile sensing of ALP in the turn-on mode, based on the simple aid by phenyl phosphate which could be hydro-lyzed by ALP, with the product of phosphate ion enhancing the FL emission of UiO-66-NH 2 via simple adsorption. Unlike many other FL probes in the turn-on mode, it was unnecessary to quench the FL of the probes in advance, greatly simplifying the sensor design. Moreover, by use of a new method based on dielectric barrier discharge (DBD), the UiO-66-NH 2 could be prepared in 10 min, much shorter than that (usually hours) for preparing most other FL probes for ALP assay. The limit of detection was 0.4 U L -1 , superior or at least rivalrous to the previously reported ones, and the ALP assay was also accomplished for real serum samples, with the analytical results highly consistent with those obtained by the clinical procedures, revealing its high practical utility.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Shusu Shen,Yang Shen,Yi Wu,Honglin Li,Chang Sun,Ganwei Zhang,Yongfu Guo
UiO-66-NH 2 is a well-known metal organic framework with high porosity and surface area, and there are modifiable reactive amino groups in its structure, it has been applied in membrane modifications. A novel composite membrane (U1gFx) is successfully prepared by depositing UiO-66-NH 2 onto polyvinylidene fluoride (PVDF) membrane, and subsequently grafting with perfluoroalkyl polyethoxy acetic acid (FPEOAA). The water contact angle of the modified membrane declines from 124.27° to 71.05°, and the under-water oil contact angle increases from 86.03° to 149.45°, indicating a good hydrophilic and oleophobic change. The modified membranes show enlarged porosity and water flux due to the introduction of UiO-66-NH 2 . The optimum membrane (U1gF10) shows excellent separation performance for various oil/water emulsions, including n -hexadecane, petroleum ether, dichloromethane and soybean oil. > 95 % oil rejection and up to 8081.9 L·m −2 ·h −1 of permeation flux are achieved under the vacuum filtration mode (0.085 MPa). While treating the n -hexadecane/water emulsion, all membranes show > 99 % oil rejection in six filtration cycles. Under a dead-end filtration mode, membrane U1gF10 gives a high relative flux recovery rate at 93 % under 0.1 MPa, its pure water flux still keeps as highly as 982.5 L·m −2 ·h −1 , even after three filtration cycles, indicating a good antifouling property and great engineering application potential.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Minjia Meng,Suao Wang,Jingyi Dai,Yi Li,Yonghai Feng,Yu Zhu,Hongbo Zhang,Yan Liu
In this work, a simple metal-organic framework (MOF) material, UiO-66-NH 2 , was prepared for the highly efficient separation of artemisinin (Art) and artesunate (Aru). Selective adsorption tests showed that UiO-66-NH 2 presented a much higher selectivity toward Aru than Art ( α Aru/Art = 40.74). The N 2 adsorption-desorption isotherm results of UiO-66-NH 2 indicated a suitable pore size to enable the free entry of Art and Aru. Contact angle analysis indicated that UiO-66-NH 2 is hydrophilic with the -NH 2 group, and can interact with the hydrophobic Aru through hydrogen bonding between the -NH 2 and -COOH groups, which is not possible with the hydrophobic Art. The selective adsorption of Aru onto UiO-66-NH 2 may be attributed to three factors: pore size, functional groups, and difference in hydrophobic/hydrophilic characteristics between the adsorbent and adsorbate. Molecularly imprinted polymers (MIPs) were prepared using Aru as a template for selective adsorption experiments to verify the excellent selectivity of UiO-66-NH 2 . The adsorption amount (65.24 mg g −1 ) and selectivity factor ( α Aru/Art = 40.74) of UiO-66-NH 2 toward Aru were significantly better than those of the MIPs (2.039 mg g −1 and 3.072, respectively). The binding capacity and better selectivity of UiO-66-NH 2 provide evidence supporting the potential of MOF adsorbents for the separation of various analogous molecules.
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