Journal of Environmental Sciences
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2022
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IF 6.796
Ping Chen,Yalan Wang,Xiaoqin Zhuang,Haijin Liu,Guoguang Liu,Wenying Lv
Zr-based metal-organic frameworks (MOFs) have been developed in recent years to treat heavy metals, e.g. hexavalent chromium Cr 6+ pollution, which damages the surrounding ecosystem and threaten human health. This kind of MOF is stable and convenient to prepare, but has the disadvantage of low adsorption capacity, limiting its wide application. To this end, a novel formic acid and amino modified MOFs were prepared, referred to as Form-UiO-66-NH 2 . Due to the modification of formic acid, its specific surface area, pore size, and crystal size were effectively expanded, and the adsorption capacity of Cr 6+ was significantly enhanced. Under optimal conditions, Form-UiO-66-NH 2 exhibited an excellent adsorption capacity (338.98 mg/g), ∼10 times higher than that reported for unmodified Zr-based MOFs and most other adsorbents. An in-depth study on the photoelectronic properties and pH confirmed that the adsorption mechanism of Form-UiO-66-NH 2 to Cr 6+ was electrostatic adsorption. After modification, the improvement of Cr 6+ adsorption capacity by Form-UiO-66-NH 2 was attributed to the expansion of its specific surface area and the increase in its surface charge. The present study revealed an important finding that Form-UiO-66-NH 2 elucidated selective adsorption to Cr 6+ in mixed wastewater containing toxic heavy metal ions and common nonmetallic water quality factors . This research provided a new acid and amino functionalization perspective for improving the adsorption capacity of Zr-based MOF adsorbents while simultaneously demonstrating their pertinence to target contaminant adsorption.
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RENEWABLE ENERGY
·
2021
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IF 8.001
Hui Li,Yongbo Wang,Xiaoling Ma,Min Guo,Yan Li,Guoning Li,Ping Cui,Shoujun Zhou,Mingzhi Yu
Ca 2+ ion leaching and poor pore structure are obstacles of CaO for biodiesel production . To this end, a typical Zr–based metal organic framework, UiO–66(Zr) is adopted to support calcium acetate to prepare CaO/ZrO 2 catalyst. For comparison, catalyst precursor is activated in nitrogen (UCN) and air (UCA) atmosphere, respectively. Preparation factors including calcium acetate addition and activation temperature are evaluated. Moreover, effects of transesterification parameters on oil conversion are investigated and the optimized parameters are further used to examine catalyst reusability . Meanwhile, catalysts are characterized with TG, XRD, XPS , FTIR, Hammett indicator titration, N 2 adsorption and desorption. Results reveal UCN calcined at 650 °C (UCN650) and UCA calcined at 700 °C (UCA700) separately exhibits the best catalytic performance. The maximum conversion of 96.99% is achieved by UCN650 with catalyst amount of 6 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min. Even after being used 3 cycles, conversion of 92.76% is still achieved by UCN650. By contrast, UCA700 shows lower conversion of 92.94% at the first cycle with catalyst amount of 8 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
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IF 3.498
He Huang,Zhao-Yang Liu,Shuang-Bao Li,Juan Zhu,Bao-Xu Jiang,Yu-Teng Zhang
In this work, an amino-functionalized Zr-based metal-organic polyhedron (denoted ZrT-1-NH 2 ), synthesised under the solvothermal method , has been selected as the photocatalyst for the removal of tetracycline (TC). The effects of adding dosages, pH values of TC degradation efficiency were investigated, and the results showed that this material was better effective in photocatalysis degradation of tetracycline antibiotic. In addition, the trapping experiments reveal that hydroxyl radical (•OH) and superoxide radical (•O 2 − ), serving as active species, play major roles in the photocatalytic process. Furthermore, a possible mechanism for the photocatalytic process is proposed. This work presents that zirconium-based metal-organic polyhedra (Zr-MOPs) may be promising photocatalysts for the removal of antibiotics in wastewater.
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FOOD CHEMISTRY
·
2023
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IF 8.8
Shitao Feng,Furong Tang,Fengshou Wu,Juan Zhang
In this study, a nanoscale Zr-based metal–organic framework (nano-Zr-MOF) was prepared by one-pot method using meso -tetra(4-carboxyphenyl)porphyrin as organic ligand and Zr 4+ as metal unit. The nanoscale structure endows it with excellent dispersion in water. The nano-Zr-MOF exhibited intense red fluorescence, which could be significantly quenched by the addition of quercetin , probably due to its electron-rich framework. The high selectivity for quercetin detection was verified with analogues and common ions as interfering agents. Moreover, the nano-Zr-MOF could be used as a highly selective and sensitive sensor for the detection of Hg 2+ . The detection limits for quercetin and Hg 2+ were 0.026 μM and 0.039 μM, respectively. This fluorometric method was successfully applied to detect quercetin in red wine and food samples with satisfactory recoveries ranging from 83.7–112.3% and 81.8–115.9%, respectively. The recovery in detection of Hg 2+ in lake water were ranging from 97.1–109.2%.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2026
·Vol. 109
·期 9
·e71223
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IF 4.2
Shenxiang Luo,Xiaopeng Hu,Junyao Wu,Qing Liu,Sai Liu,Jinwei Guo,Fan Zhang,Wang Zhu
A series of A 6 Ta 2 O 17 /8YSZ double-ceramic-layer thermal barrier coatings (TBCs) with varying Hf/Zr molar ratios (1:2, 1:1, and 2:1) are fabricated via atmospheric plasma spraying (APS). The effect of the Hf/Zr ratio on the microstructure, mechanical properties, and high-temperature performance of the coatings under both thermal cycling and thermal shock conditions is systematically investigated. As Hf content increases, the nano-hardness decreases markedly from 16.5 to 12.8 GPa, whereas the intrinsic elastic modulus shows a modest increase from 222.8 to 232.8 GPa. Concurrently, the interfacial fracture toughness decreases from 0.96 to 0.62 MPa·m 1/2 . The equimolar H1Z1 coating (Hf/Zr = 1:1) demonstrates the highest thermal cycling resistance (2371 cycles), a performance attributed to a failure mechanism involving multi-channel stress release at the interfaces. Under thermal shock conditions, the H1Z1 coating also exhibits a prolonged thermal shock lifetime of 2180 cycles. In contrast, the Hf-rich composition (Hf/Zr = 2:1) fails catastrophically after only 682 cycles, due to insufficient erosion resistance, marked by pit formation and progressive thinning. These results highlight the equimolar H1Z1 coating as offering an optimal balance of mechanical compatibility and service durability, making it the most promising candidate among the investigated compositions for advanced TBCs applications.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 41
·16033-16045
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IF 4.5
Tian Yuhao,Li Ting,Cai Weijie
Recently, bio-ethanol reforming with CO 2 (EDR) has been considered as one of the environment-friendly processes to diminish the emission of greenhouse gas, along with increasing the production of value-added syngas. However, designing high-performance catalysts is still a great challenge. In this work, MOF-derived CoMO x (M:Ce,Zr,Zn) catalysts were applied in EDR reaction for the first time to explore the influence of support types on catalytic performance. Characterization of the investigated catalysts by XPS, XRD, H 2 -TPR, Raman, TEM and BET depicted the difference in cobalt dispersion, specific surface area as well as Co-support interaction. Indeed, H 2 -TPR and XPS results revealed stronger Co-Ce interaction and the smaller particle size of Co 3 O 4 in Co-CeO 2 catalyst which contributed to higher activity. Indeed, 100% of ethanol conversion was obtained at 550 °C and the formed H 2 /CO ratio (1.18) was suitable for the downstream Fischer–Tropsch process. Meanwhile, no remarkable decline of ethanol conversion and product distributions occurred after 40 h stability tests. The findings implied that EDR process might be suitable to consume greenhouse gas and reduce carbon footprint. Characterization results of the used catalysts indicated that Co-CeO 2 catalyst presented an outstanding anti-aggregation and anti-coking property. Herein, the effect of support type in this work might provide guidance for the design of high-performance catalysts for other heterogeneous reactions operated at high temperature. Graphical abstract
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Journal of Physical Chemistry C
·
2023
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IF 3.7
Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang
The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Li Wang,Yi Pan,Zhengwu Wang,Yuanfeng Wang,Xinlin Wei
Organophosphorus pesticides (OPPs) are extensively used in agricultural production, and the contamination caused by their residues has raised significant concerns regarding potential threats to human health. Herein, a novel fluorescence nanoprobe based on an enzyme-mediated silver nanoparticle-modified metal organic framework (AgNPs@PCN-224) was successfully prepared for the rapid detection of OPPs. Initially, AgNPs@PCN-224 were synthesized by reducing silver nitrate (AgNO3) using sodium borohydride (NaBH4) embedded into luminescent PCN-224. This triggered the inner filter effect, leading to fluorescence quenching. Meanwhile, under the catalysis of acetylcholinesterase (AChE) and choline oxidase (CHO), acetylcholine (ATCh) was decomposed to hydrogen peroxide (H2O2), which could destroy AgNPs to form Ag+ released from PCN-224 for fluorescence recovery. Instead, fenitrothion, an OPP, inhibited AChE activity, allowing the quenched fluorescence to be reactivated. Under the current optimum conditions, the fluorescence intensity had a good correlation (Y = −728.5370X + 2178.4248, R2 = 0.9869) over a dynamic range of fenitrothion concentrations from 0.1 to 500 ng/mL, with an LOD of 0.037 ng/mL. In addition, the anti-interference ability and robustness of the proposed sensor was verified for the monitoring of fenitrothion in tea with recoveries of 87.67–103.72% and the relative standard deviations (RSD) < 5.43%, indicating that the system has excellent prospects for OPP determination in practical applications. Furthermore, this work provides a universal platform for screening other enzyme inhibitors to detect OPPs.
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International Journal of Electrochemical Science
·
2023
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IF 1.5
Yong Chang,Fengli Gao,Tong Wu,Qiuzhi Pan,Lin Liu,Qijun Song
Protein kinases play a vital regulatory role in various biological processes. In this work, we developed an electrochemical biosensor for the detection of protein kinases using methylene blue (MB)-functionalized Zr-based metal-organic frameworks (MOFs, UiO-66-NH 2 ) as the signal labels. The results of UV-Vis spectroscopy, X-ray diffraction and N 2 adsorption–desorption experiments confirmed the successful encapsulation of MB into UiO-66-NH 2 . The phosphate groups in phosphorylated peptides were recognized by UiO-66-NH 2 via the robust coordination with Zr-O clusters on the surface of MOFs. The encapsulated MB molecules in UiO-66-NH 2 produced a strong electrochemical signal for highly sensitive detection of protein kinases, which was recorded by square wave voltammetry (SWV). With protein kinase A (PKA) as a model target, the biosensor achieved a detection limit of 0.02 U/mL and a linear range from 0.05 to 20 U/mL. The proposed biosensor was utilized to screen potential inhibitors and determine PKA in serum samples with satisfactory results. This work provided an effective strategy for electrochemical assays of phosphorylation-related biological events in clinical diagnosis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Zhou Fang,Zheng Deng,Xinyi Wan,Zhuoyi Li,Xu Ma,Shabab Hussain,Zhizhen Ye,Xinsheng Peng
Although Keggin-type polyoxometalates (POMs) have shown nice catalytic efficiency for CO 2 cycloaddition reaction, they suppressed by their low recycling ability and energy costing of direct heating. Decorated POMs into solid porous support with photothermal property is an alternative but promising way for solar-driven reaction. Herein, phosphomolybdate molecularly decorated ferrocene-based Zr-Fc (PMo 12 @Zr-Fc) metal organic frameworks (MOFs) nanosheet, which has outstanding photothermal conversion ability, are synthesized and used to catalyze cycloaddition reaction with styrene oxide and CO 2 under simulated sunlight. At light intensity of 0.4 W/cm 2 , the temperature of reactor with PMo 12 @Zr-Fc MOFs rapidly rises and up to 80 ℃, and 88.05 % yield of product is achieved. This PMo 12 @Zr-Fc catalyst also demonstrates nice recycling stability. The solar-driven cycloaddition process may exploit a new avenue for reusing CO 2 .
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ACS Applied Materials & Interfaces
·
2020
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IF 8.758
Zheng Deng,Chao Fang,Xu Ma,Xiang Li,Yu-Jia Zeng,Xinsheng Peng
Metal–organic frameworks (MOFs) have been identified as promising materials for the delivery of therapeutics to cure cancer owing to their intrinsic porous structure. However, in a majority of cases, MOFs act as only a delivery cargo for anticancer drugs while little attention has been focused on the utilization of their intriguing physical and chemical properties for potential anticancer purposes. Herein for the first time, an ultrathin (16.4 nm thick) ferrocene-based MOF (Zr-Fc MOF) nanosheet has been synthesized for synergistic photothermal therapy (PTT) and Fenton reaction-based chemodynamic (CDT) therapy to cure cancer without additional drugs. The Zr-Fc MOF nanosheet acts not only as an excellent photothermal agent with a prominent photothermal conversion efficiency of 53% at 808 nm but also as an efficient Fenton catalyst to promote the conversion of H2O2 into hydroxyl radical (•OH). As a consequence, an excellent therapeutic performance has been achieved in vitro as well as in vivo through this combinational effect. This work aims to construct an “all-in-one” MOF nanoplatform for PTT and CDT treatments without incorporating any additional therapeutics, which may launch a new era in the investigation of MOF-based synergistic therapy platforms for cancer therapy.
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ANALYTICA CHIMICA ACTA
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2020
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IF 5.977
Zhengjie Hu,Ximing Wang,Xuwei Chen
Highly selective adsorption of protein species interested from complicated biological samples is an extremely important prerequisite for in-depth proteomic analysis. Herein, a novel dual-hydrophilic material is fabricated by grafting Zr-based metal-organic framework (Zr-MOF) onto the surface of magnetic microspheres , and subsequent modifying with fructose-1,6-bisphosphate (FBP) molecules by taking advantage of multivalent binding between the phosphate backbone of FBP and Zr centers. Owing to the favorable dual-hydrophilicity derived from the abundant amino groups in Zr-MOF and the hydroxyl groups in FBP molecules, the obtained magnetic microspheres (mMOF-FBP) provide high adsorption efficiency, favorable selectivity and excellent capturing capacity (555.6 mg g −1 ) towards immunoglobulin G (IgG). The captured IgG could be collected from the mMOF-FBP by using 0.5% (m/v) NH 3 ·H 2 O as elution reagent with a recovery of 88.4%. The dual-hydrophilic microspheres demonstrate their practicability by selective isolation of IgG from human serum.
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