ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Xuanhe Hu,Tian Huang,Shipeng Wang,Shangjun Lin,Zihao Feng,Lai-Hon Chung,Jun He
The shuttle effect of soluble polysulfides as one of the primary bottlenecks has retard the widespread use of lithium-sulfur (Li-S) batteries. In this work, a new functional separator coating composed of pristine zirconium metal-organic framework (Co-PCN-222) with catalytic cobalt-porphyrin linker decorated carbon nanotubes (PCN@CNT) was presented for addressing this problem. Benefiting from powerful adsorption and catalytic activity of the uniformly dispersed cobalt and nitrogen sites in porphyrin linkers as well as the fast electron transport network provided by highly conductive CNT, the polysulfide redox kinetics is greatly boosted and the shuttle effect is inhibited to a large extent. Accordingly, the Li-S batteries coupling with PCN@CNT coated separator delivers a specific capacity as high as 1157 mAh g −1 at 0.1 C, good rate capability with a reversible capacity of 696 mAh g −1 under 2 C as well as excellent cyclic performance with a low average capacity attenuation rate of 0.067% upon 500 cycles at 1 C. This work will open up great opportunities in the development of pristine MOFs-based separator coating for advanced Li-S batteries.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6556
·
IF 4.105
Wen-Jing Qiu,Ming-Wu Gao,Qi Chen,Ao Zheng,Yi-Jia Shi,Xin Liu,Juan-Hong Li,Guo-Liang Dai,Yang Hu,Zi-Xia Lin
Under normal temperature and pressure, a novel improved Fenton system that was named MHACF-MOF-808(Zr) was constructed after the introduction of Pd/MOF-808(Zr) and H 2 to solve the inherent problem of the production of iron sludge in the classic Fenton system. Only trace amount of Fe II was required during the whole reaction because Fe III could be rapidly reduced by the active hydrogen derived from the adsorption and activation of H 2 on the surface of Pd/MOF-808(Zr) composite. The concentration of Fe II could be maintained more than 10 μM. The removal of target pollutant sulfamethazine in this system was mainly relied on the degradation of ·OH verified by both of the direct detection and indirect inhibition (using methanol). By using the calculation of Laplacian bond order, the degradation pathway of sulfamethazine followed by the cleavage of N S bond. This prediction was verified by the detection of intermediate products. Only 21% sulfamethazine could be degraded after 3-h reaction in the classic Fenton reaction system, while it could be thoroughly degraded in 1.5 h in the MHACF-MOF-808(Zr) system. The influence of main parameters on the degradation effect of sulfamethazine, such as initial pH, the flow of H 2 , dosage of Pd/MOF-808(Zr), concentration of sulfamethazine, ferrous, and hydrogen peroxide, were systematically studied. Based on the relative stability of Pd/MOF-808(Zr) confirmed by the morphological characterization, sulfamethazine could be efficiently degraded in the MHACF-MOF-808(Zr) system.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jian Chen,Jinbo Ouyang,Wenqian Chen,Zepeng Zheng,Zhen Yang,Zhirong Liu,Limin Zhou
Porous chitosan/Zr-MOF (UiO-66) composite foams (CSF@UiO-66) were facilely prepared by grafting UiO-66 into polymerized chitosan using epichlorohydrin as the linking agent. The flexible foams with high loadings of UiO-66 exhibited low density (15.0 ∼ 23.4 mg/cm 3 ) and superior liquid–solid separation performance. The hierarchical pores and abundant functional groups contributed to the effective removal of ketoprofen (KPF) from water by the composite foams, achieving a maximum adsorption capacity of 209.7 mg/g at pH 4, outperforming most reported adsorbents. Batch adsorption experiments demonstrated that the adsorption of KPF could be described by the Langmuir isotherm and pseudo-second-order kinetic model. Importantly, the composite foams showed excellent performance even in the presence of some ions and good reusability for engineering applications. Furthermore, density functional theory (DFT) calculations revealed that the adsorption mechanism between the composite foams and KPF could be attributed to hydrogen bonding and π-π interaction. In essence, this work provides an innovative strategy for the fabrication of a blocky composite foam with high loadings of MOF for efficient adsorptive removal of KPF in liquids, which can overcome the disadvantages of agglomeration due to small particle size and poor stability of MOFs.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 18
·8045-8053
·
IF 3.591
Yaping Zhang,Daofei Lv,Jiayu Chen,Zewei Liu,Chongxiong Duan,Xin Chen,Wenbing Yuan,Hongxia Xi,Qibin Xia
The separation of ethylene/ethane mixtures using energy-efficient technologies is important but challenging. In this study, we prepared a Zr-based metal–organic framework (MOF-545) possessing a high Brunauer–Emmett–Teller (BET) surface area of 2265.4 m2 g−1, and investigated its adsorption performance for ethylene/ethane separation. Isotherm measurements show that MOF-545 exhibits preferential adsorption of ethane over ethylene. The mechanism underlying the selective adsorption of ethane over ethylene was revealed by the calculations of preferential adsorption sites, interaction energies and adsorption density distributions of ethane and ethylene in MOF-545 via the Metropolis Monte Carlo method. Results show that the strong C–H⋯N hydrogen bonding between ethane molecules and porphyrin rings gives rise to the selective adsorption of ethane over ethylene. Thermal, air and cycling stability tests, adsorption selectivity and adsorption enthalpy calculations, and breakthrough experiments comprehensively validate the potential of MOF-545 as an efficient ethane-selective adsorbent for ethane/ethylene separation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chen Wang,Chao Xiong,Yali He,Chen Yang,Xiteng Li,Jianzhong Zheng,Shixing Wang
A novel magnetic Zr-MOF named Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI was synthesized by modifying UiO-66-NH 2 with Ni 0.6 Fe 2.4 O 4 and polyethyleneimine and its sorption characteristics for two representing heavy metals Pb(II) and Cr(VI) in water were examined. This material showed good thermal stability and was sufficiently magnetic to allow effective solid-liquid separation. The material had a maximum adsorption capacity of 273.2 mg/g for Pb(II) at pH 4.0 and 428.6 mg/g for Cr(VI) at pH 3.0, as obtained from the model fitting by the Hill equation. The sorption kinetics for both heavy metals on the material was fast, with adsorption equilibrium established in 60 min and 30 min for Pb(II) and Cr(VI), respectively. Model fitting of the kinetic data showed that Pb(II) and Cr(VI) sorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI followed the pseudo-second-order model. This material had good selectivity for competing ions, and still hold fairly good binding capacities after 5 times of regeneration. Adsorption mechanisms for Pb(II) and Cr(VI) by Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI were proposed by analyzing FTIR, XPS and the electrokinetic property of the material. Specifically, Pb(II) adsorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be attributed to chelation of Pb(II) with the imine/amine functional groups in the material’s matrix, while Cr(VI) adsorption might stem from a combination of electrostatic attraction, chelation and redox reaction. It seems that Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be used as a green and environmental-friendly material for heavy metals removal, particularly from acidic water streams.
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RSC Advances
·
2020
·Vol. 10
·期 33
·19149-19156
·
IF 3.119
Liu Yang,Yu-Long Liu,Cheng-Guo Liu,Ying Fu,Fei Ye
A RhB@Zr-MOF composite with dual-emission properties was successfully constructed, which comprises a zirconium-based metal–organic framework and the luminescent dye molecule, Rhodamine B (RhB), embedded via the encapsulation method. The fluorescence intensity ratio of the two emissions was found to be ca. 370 nm/590 nm for RhB@Zr-MOF. The fluorescence intensity values of the two emissions of RhB@Zr-MOF can also be affected by the structures of analytes containing different organic groups. Due to the existence of the dual-emission properties in RhB@Zr-MOF, the relative fluorescence intensity of the emission peaks was introduced as a detection index instead of absolute fluorescence intensity. RhB@Zr-MOF, which possesses the characteristics of a built-in self-calibrating fluorescence sensor, was investigated for detecting cations, nitroaromatics and pesticides. Aside from high sensitivity and selectivity, recyclability is the most important property for sensing pesticides. This work shows that RhB@Zr-MOF can maintain its stability after 5 cycles of detecting nitenpyram, with LOD of 0.2 μM. These results demonstrate that dye@MOFs with dual-emission properties can be employed as multifunctional fluorescence sensors for different types of analytes, and that RhB@Zr-MOF provides a new paradigm for analyte sensing.
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ENERGY & FUELS
·
2020
·
IF 3.421
Junhua Zhang,Zhaohua Qi,Yao Liu,Junnan Wei,Xing Tang,Liang He,Lincai Peng
Catalytic transfer hydrogenation (CTH) of 5-hydroxymethylfurfural (HMF) into 2,5-bis(hydroxymethyl)furan (BHMF) is an important method for the catalytic upgrading of biomass-derived platform compounds to fuels and chemicals, and the development of effective and economical catalysts for this purpose is of great significance. In this work, we designed and prepared a new carbon-nanosheets (CNS)-supported Zr/Ca bimetallic catalyst (ZrCa@CNS) with low cost by a “gel-blowing” strategy. Comprehensive studies revealed that ZrCa(2)@CNS-600 exhibited good catalytic activity on the CTH of HMF into BHMF via Meerwein–Ponndorf–Verley (MPV) reduction, and an 84.2% BHMF yield with a 91.2% HMF conversion was obtained in isopropyl alcohol at 190 °C in 10 h. ZrCa(2)@CNS-600 exhibited good heterogeneity, reusability, and stability, and it is readily recovered from the reaction mixture by filtration and consecutively recycled/reused for six times without an obvious loss in its catalytic activity.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Liangqiong Ren,Feng Hong,Lingwen Zeng,Yiping Chen
To address the urgent demand for sensitive and stable detection applications, significant efforts have been made in the development of dual-signal readout assays for precise target detection and timely health risk control. Here, a new nanomaterial, Pt@PCN-224-HRP-initiator DNA (PP-HRP-iDNA), was exploited to construct a dual-signal readout biosensing platform. Zr-MOF (PCN-224) was loaded with as many Pt nanoparticles (NPs) and as much horseradish peroxidase (HRP) as possible to enhance the brightness of the colorimetric signal recognizable to the naked eye while also acting as a gatekeeper to protect the enzyme activity and ensuring the stability of the assay process. Moreover, the Pt NPs and HRP displayed a synergistic catalytic effect, which promoted the sensitivity of detection. Further, the formation of the Zr–O–P bond eliminated the instability of the interactions between PCN-224 and iDNA in a controllable manner. After the immunoreaction, iDNA stimulated a hybridization chain reaction, resulting in a significant reduction of the fluorescent DNA in the supernatant and a fluorescent signal change. Subsequently, the PP-HRP-iDNA probe implemented UV-light response (450 nm) where 3,3′,5,5′-tetramethylbenzidine was used as a substrate for the colorimetric signal readout. By virtue of the nanomaterial-modulated transduction mechanism and the antigen–antibody interactions, this dual-signal biosensor displays high sensitivity, with a limit of detection of 0.65 pg/mL for aflatoxin B1 and 4 CFU/mL for Salmonella enteritidis, suggesting the detection potential of the biosensing platform for analyzing various targets.
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Journal of Analysis and Testing
·
2026
·
IF 9.4
Huang Shan,Liu Xinqi,Huang Aoxiang,Zhuo Yongxiu,Huang Tiantian,Fang Yi,Wei Fuxiang,Xiao Qi
As one of the most extensively applied herbicides globally, glyphosate (GLY) is frequently detected in food and water matrices, raising substantial concerns regarding its potential harm to human health. Addressing this challenge calls for analytical platforms that offer both reliable performance and operational convenience. In this work, a GLY-responsive nanoenzyme was developed by hybridizing Zr-based metal–organic frameworks (Zr-MOF) with manganese dioxide (MnO 2 ). The system capitalizes on the strong chelation between GLY and metal centers, which destabilizes the nanozyme structure and consequently modulates its catalytic activity toward colorimetric readout. The resulting composite enables precise quantification of GLY in solution and can be readily incorporated into paper substrates to support visual, user-friendly sensing. In solution format, the assay achieves a linear response over 0.001–10 mg/mL with a limit of detection (LOD) of 0.9 μg/mL, whereas the paper-based counterpart operates within 0.05–20 mg/mL and affords an LOD of 0.03 mg/mL, making it well-suited for cost-effective field applications. Both detection formats were validated using GLY-spiked fruit and water samples. Recovery rates fell between 90.5% and 110% for the solution-based method, and between 95.3% and 105% for the paper-based strips, with relative standard deviations (RSDs) of less than 15% and 7%, respectively, indicating satisfactory accuracy and reproducibility. Overall, this work presents a versatile strategy that bridges high analytical precision with straightforward operation, meeting the demands of both routine monitoring and point-of-use testing by non-professionals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiajun Yu,Xiao Wang,Yan Wang,Xiaofeng Xie,Haijiao Xie,Nat Vorayos,Jing Sun
The removal of indoor/outdoor toluene by photocatalysis has drawn much attention due to its low energy consumption and easy availability. However, light inevitably generates heat, and pollutants desorb from catalysts as the temperature rises, which is not beneficial to degradation. Contrast to the frequently occurred phenomena, we firstly found that the adsorption capacity of UiO-66 (Zr) on toluene increased with increasing temperature as adsorption isotherms and in-situ Fourier transform infrared spectra (in-situ FTIR) showed. The optimum temperature was 30 °C. This stage in which adsorption capacity was positively correlated with temperature was called heating-induced adsorption, which achieved a toluene removal efficiency of 69.6 %. By density functional theory (DFT) calculations and changing the metal centers and organic ligands of UiO-66 (Zr) respectively, we disclosed that the heating-induced adsorption was mainly related to the π-π stacking interaction of MOF ligands and toluene. The analysis of samples before and after adsorption showed that the interaction between UiO-66 (Zr) and adsorbed toluene facilitated the charge transfer and prolonged the carrier lifetime, leading to the increase of hydroxyl radicals (•OH) in photocatalysis. Therefore, a synergistic effect between heating-induced adsorption and photocatalysis was proposed by analyzing the adsorption of toluene on UiO-66 (Zr) in detail. This work provided new viewpoint to understand the role of concomitant heat contributed to the adsorption and degradation of toluene during photocatalysis.
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Small
·
2023
·Vol. 19
·期 36
·2302357
·
IF 13.3
Zhilin Li,Mengyan Cao,Zhihui Rao,Xiujian Zhao,Xiao Gong
Low-dimensional hybrid metal halide (LDHMH) materials have attracted considerable attention owing to their intriguing optical properties. To the best of the knowledge, this is the first study to successfully demonstrate both self-trap exciton (STE) and afterglow emissions in Zr-based LDHMH materials. The obtained pure (Ph 3 S) 2 ZrCl 6 crystals showed near-ultraviolet phosphorescence and a green afterglow owing to the organic cation Ph 3 S + , while the Bi-doped and Sb-doped crystals exhibited both STE and afterglow emissions. However, the Te-doped crystals showed only a broad yellow STE emission owing to the [TeCl 6 ] 2− octahedron. In addition, all the crystals showed good stability. Notably, Sb-doped crystals produced white light, which can be adjusted between cold white and warm white using different excitations. Finally, this strategy for both STE and afterglow emissions can be applied to other LDHMH materials for optical applications.
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MOLECULES
·
2023
·Vol. 28
·期 7
·2923
·
IF 4.6
Enmin Zong,Xuanren Wang,Lirong Zhang,Jiayao Yang,Xiaohuan Liu
The application of lignin-based adsorbents in the efficient removal of phosphate from wastewater has attracted much attention and been intensively studied in recent years. However, most currently reported lignin-based adsorbents are difficult to recover and recycle. Herein, we have developed a recyclable, nanostructured bio-adsorbent, poly(ethyleneimine) (PEI)-modified lignin (LG) integrated with Fe3O4and Zr-La dual-metal hydroxide (LG-NH2@Fe3O4@Zr-La), by the Mannich reaction followed by the chemical coprecipitation method. Multilayer adsorption existed on the surface of LG-NH2@Fe3O4@Zr-La based on the isotherm fitting curve, and its adsorption capacity reached 57.8 mg P g−1, exhibiting a higher phosphate uptake than most reported metallic oxide-based composites. The adsorption process was dominated by inner-sphere complexation of ligand-exchange and electrostatic interactions. Moreover, LG-NH2@Fe3O4@Zr-La exhibited excellent selectivity against coexisting anions, and the adsorption was more efficient under acidic conditions. When the phosphate concentration was 2.0 mg P L−1, the removal efficiency of phosphate reached 99.5% and the residual concentration was only 10 μg P L−1, which meets the United States Environmental Protection Agency (USEPA) standard for eutrophication prevention. In addition, the LG-NH2@Fe3O4@Zr-La displayed excellent reusability, maintaining 91.8% of removal efficiency after five cycles. Importantly, owing to the magnetic properties of the loaded Fe3O4, the resulting composite could be separated within 30 s under an external magnetic field. Thus, the separable and recyclable biobased magnetic adsorbent developed in this work exhibited promising application in phosphate capture from real sewage. This research study provides a new perspective for lignin valorization in lignocellulose biorefineries and establishes an approach for developing an economical and efficient bio-adsorbent for phosphate removal from wastewater.Keywords:lignin;magnetic adsorbent;Zr hydroxides;La hydroxides;phosphate;recycle
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