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1.
J Environ Sci (China) ; 148: 174-187, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095155

RESUMO

Cost-effective CO2 adsorbents are gaining increasing attention as viable solutions for mitigating climate change. In this study, composites were synthesized by electrochemically combining the post-gasification residue of Macadamia nut shell with copper benzene-1,3,5-tricarboxylate (CuBTC). Among the different composites synthesized, the ratio of 1:1 between biochar and CuBTC (B 1:1) demonstrated the highest CO2 adsorption capacity. Under controlled laboratory conditions (0°C, 1 bar, without the influence of ambient moisture or CO2 diffusion limitations), B 1:1 achieved a CO2 adsorption capacity of 9.8 mmol/g, while under industrial-like conditions (25°C, 1 bar, taking into account the impact of ambient moisture and CO2 diffusion limitations within a bed of adsorbent), it reached 6.2 mmol/g. These values surpassed those reported for various advanced CO2 adsorbents investigated in previous studies. The superior performance of the B 1:1 composite can be attributed to the optimization of the number of active sites, porosity, and the preservation of the full physical and chemical surface properties of both parent materials. Furthermore, the composite exhibited a notable CO2/N2 selectivity and improved stability under moisture conditions. These favorable characteristics make B 1:1 a promising candidate for industrial applications.


Assuntos
Dióxido de Carbono , Estruturas Metalorgânicas , Dióxido de Carbono/química , Adsorção , Estruturas Metalorgânicas/química , Poluentes Atmosféricos/química , Carvão Vegetal/química
2.
Angew Chem Int Ed Engl ; : e202409256, 2024 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-39088255

RESUMO

Developing an anode material that has better performance efficiency than commercial graphite while keeping the features of economic scalability and environmental safety is highly desirable yet challenging. MOFs are a promising addition to the ongoing efforts, however, the relatively poor performance, chemical instability, and large-scale economic production of efficiency-proven pristine MOFs restrict their utility in real-life energy storage applications. Furthermore, hierarchical porosity for lucid mass diffusion, high-density lithiophilic sites are some of the structural parameters for improving the electrode performance. Herein, we have demonstrated the potential of economically scalable salicylaldehydate 3D-conjugated-MOF (Fe-Tp) as a high-performance anode in Li-ion batteries: the anode-specific capacity achieved up to 1447 mA h g-1 at 0.1 A g-1 and 89% of cyclic stability after 500 cycles at 1.0 A g-1.for pristine MOF. More importantly, incorporating 10% Fe-Tp doping in commercial graphite (MOFite) significantly enhanced lithium storage, doubling capacitance after 400 cycles. It signifies the potential practical utility of Fe-Tp as a performance booster for commercial anode material.

3.
Food Chem ; 460(Pt 2): 140660, 2024 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-39089029

RESUMO

This study utilized computational simulation and surface molecular imprinting technology to develop a magnetic metal-organic framework molecularly imprinted polymer (Fe3O4@ZIF-8@SMIP) capable of selectively recognizing and detecting multiple fluoroquinolones (FQs). The Fe3O4@ZIF-8@SMIP material was synthesized using the "common" template-ofloxacin, identified by computational simulation, demonstrating notable adsorption capacity (88.61-212.93 mg g-1) and rapid mass-transfer features (equilibration time: 2-3 min) for all tested FQs, consistent with Langmuir adsorption model. Subsequently, this material was employed as a magnetic solid-phase-extraction adsorbent for adsorption and detection of multiple FQs by combining with high performance liquid chromatography. The developed method exhibited good linearity for various FQs within the concentration range of 0.1-500 µg L-1, with low limit of detection (0.0605-0.1529 µg L-1) and limit of quantitation (0.2017-0.5097 µg L-1). Satisfactory recoveries (88.38-103.44%) were obtained when applied to spiked food samples, demonstrating the substantial potential of this Fe3O4@ZIF-8@SMIP material for rapid enrichment and identification for multiple FQs residues.

4.
Small ; : e2405051, 2024 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-39092657

RESUMO

Metal-organic frameworks (MOFs)-related Cu materials are promising candidates for promoting electrochemical CO2 reduction to produce valuable chemical feedstocks. However, many MOF materials inevitable undergo reconstruction under reduction conditions; therefore, exploiting the restructuring of MOF materials is of importance for the rational design of high-performance catalyst targeting multi-carbon products (C2). Herein, a facile solvent process is choosed to fabricate HKUST-1 with an anionic framework (a-HKUST-1) and utilize it as a pre-catalyst for alkaline CO2RR. The a-HKUST-1 catalyst can be electrochemically reduced into Cu with significant structural reconstruction under operating reaction conditions. The anionic HKUST-1 derived Cu catalyst (aHD-Cu) delivers a FEC2H4 of 56% and FEC2 of ≈80% at -150 mA cm-2 in alkaline electrolyte. The resulting aHD-Cu catalyst has a high electrochemically active surface area and low coordinated sites. In situ Raman spectroscopy indicates that the aHD-Cu surface displays higher coverage of *CO intermediates, which favors the production of hydrocarbons.

5.
Adv Mater ; : e2408094, 2024 Aug 03.
Artigo em Inglês | MEDLINE | ID: mdl-39096074

RESUMO

Multinuclear metal clusters are ideal candidates to catalyze small molecule activation reactions involving the transfer of multiple electrons. However, synthesizing active metal clusters is a big challenge. Herein, on constructing an unparalleled Co4(SO4)4 cluster within porphyrin-based metal-organic frameworks (MOFs) and the electrocatalytic features of such Co4(SO4)4 clusters for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is reported. The reaction of CoII sulfate and metal complexes of tetrakis(4-pyridyl)porphyrin under solvothermal conditions afforded Co4-M-MOFs (M═Co, Cu, and Zn). Crystallographic studies revealed that these Co4-M-MOFs have the same framework structure, having the Co4(SO4)4 clusters connected by metalloporphyrin units through Co─Npyridyl bonds. In the Co4(SO4)4 cluster, the four CoII ions are chemically and symmetrically equivalent and are each coordinated with four sulfate O atoms to give a distorted cube-like structure. Electrocatalytic studies showed that these Co4-M-MOFs are all active for electrocatalytic OER and ORR. Importantly, by regulating the activity of the metalloporphyrin units, it is confirmed that the Co4(SO4)4 cluster is active for oxygen electrocatalysis. With the use of Co porphyrins as connecting units, Co4-Co-MOF displays the highest electrocatalytic activity in this series of MOFs by showing a 10 mA cm-2 OER current density at 357 mV overpotential and an ORR half-wave potential at 0.83 V versus reversible hydrogen electrode (RHE). Theoretical studies revealed the synergistic effect of two proximal Co atoms in the Co4(SO4)4 cluster in OER by facilitating the formation of O─O bonds. This work is of fundamental significance to present the construction of Co4(SO4)4 clusters in framework structures for oxygen electrocatalysis and to demonstrate the cooperation between two proximal Co atoms in such clusters during the O─O bond formation process.

6.
Adv Mater ; : e2309572, 2024 Aug 03.
Artigo em Inglês | MEDLINE | ID: mdl-39096076

RESUMO

The construction of ultrathin porous membranes with stable structures is critical for achieving efficient gas separation. Inspired by the binary-cooperative structural features of bones and teeth-composed of rigid hydroxyapatite and flexible collagen, which confer excellent mechanical strength-a binary-cooperative porous membrane constructed with gel-state zeolitic imidazolate frameworks (g-ZIFs), synthesized using a metal-gel-induced strategy, is proposed. The enlarged cavity size and flexible frameworks of the g-ZIF nanoparticles significantly improve gas adsorption and diffusion, respectively. After thermal treatment, the coordination structures forming rigid segments in the g-ZIF membranes appear at the stacked g-ZIF boundaries, exhibiting a higher Young's modulus than the g-ZIF nanoparticles, denoted as the flexible segments. The g-ZIF membranes demonstrate excellent tensile and compression resistances, attributed to the effective translation of binary-cooperative effects of rigidity and flexibility into the membranes. The resulting dual-aperture structure, composed of g-ZIF nanoparticles surrounded by nanoscale apertures at the boundaries, yields a membrane with a stable CO2 permeance of 4834 GPU and CO2/CH4 selectivity of 90 within 3.0 MPa.

7.
Food Chem ; 460(Pt 3): 140690, 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39106752

RESUMO

The misuse of tetracyclines in livestock production poses significant health risks. Thus, establishing convenient detection methods to replace complex laboratory tests for food safety is crucial. In this study, a heterostructure Zn-BTC/IRMOF-3 (denoted as ZBI) asynchronous response fluorescence sensor was developed for the qualitative and quantitative detection of tetracyclines in foods. The ZBI solution exhibited blue fluorescence under UV excitation; upon the introduction of tetracyclines, ZBI selectively recognized the tetracycline molecules through electron transfer, π-π stacking, and chelation, resulting in blue fluorescence quenching and green fluorescence enhancement. The ZBI sensor for tetracycline detection achieved recovery rates ranging from 93.91 to 111.91% in food samples, with a detection limit of as low as 0.086 µmol/L. Lastly, a portable sensing device using support vector classifier was constructed for detecting tetracyclines in real-life scenarios. Our findings introduce a new approach for fabricating fluorescence sensors and offer a novel method for detecting tetracyclines.

8.
J Colloid Interface Sci ; 677(Pt A): 502-511, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39106775

RESUMO

Metal-organic framework (MOF) derivatives with tunable pore structure and improved conductivity are intensively designed as electroactive materials. Incorporating structure directing agents (SDA) is beneficial for designing MOF derivatives with excellent electrochemical performances. Ammonium fluoroborate has been reported as an effective SDA, coupled with cobalt salt and 2-methylimidazole, to synthesize zeolitic imidazolate framework-67 (ZIF-67) derivatives for charge storage. However, the synthetic environment for growing cobalt-based active materials is relatively complex. In this study, cobalt tetrafluoroborate (Co(BF4)2) is proposed as a novel cobalt precursor, supplementing cobalt ions and acting as the SDA in a single chemical, to synthesize the cobalt-based electroactive material of energy storage electrodes. Interactions between solvent molecules and solutes play significant roles on the morphology, composition, and electrochemical performance of active materials. Deionized water, methanol and ethanol are used as precursor solvents to understand their effects on material and electrochemical properties. The optimal electrode presents a specific capacitance of 608.3 F/g at 20 mV/s, attributed to the highest electrochemical surface area and evident compositions of cobalt fluoride and hydroxide. A battery supercapacitor hybrid achieves the maximum energy density of 45 Wh/kg at 429 W/kg. The CF retention of 100% and Coulombic efficiency of 99% are achieved after 10,000 cycles.

9.
Luminescence ; 39(8): e4859, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39108165

RESUMO

Chlorpyrifos (CPS) is widely found in food and water sources due to agricultural use, posing health and environmental risks. Therefore, this work introduces a fluorescent sensor design of silver nanoparticle-embedded nano zirconium-based metal-organic frameworks (UiO-66-NH2@AgNPs) for accurate examination of CPS. Briefly, UiO-66-NH2 was synthesized hydrothermally, exhibiting weak luminescence owed to ligand-to-metal charge transfer (LMCT). Here, it limits its direct utility in fluorescence-based detection. To address this limitation, silver nanoparticles (AgNPs) were introduced into UiO-66-NH2, enhancing fluorescence via the metal-enhanced fluorescence (MEF) effect. Briefly, a comprehensive spectral analysis such as XPS, SEM, TEM, PXRD, etc., was performed to validate the synthesis of UiO-66-NH2@AgNPs. Subsequent evaluation revealed that CPS effectively quenched the luminescence intensity of UiO-66-NH2@AgNPs through a static quenching mechanism. The fluorescence intensity exhibited good linearity with CPS concentration in the span of 10 to 1,000 ng/mL, with a recognition limit of 191.5 ng/mL(S/N = 3). The interaction involved Ag-S bond formation and electrostatic interactions, reducing fluorescence intensity. The method was confirmed through successful CPS detection in fruit samples. The UiO-66-NH2@AgNPs nanoprobe offers a simple, sensitive, and accurate platform for CPS sensing, with potential for future use in detecting CPS in fruits and vegetables.


Assuntos
Clorpirifos , Nanopartículas Metálicas , Estruturas Metalorgânicas , Prata , Zircônio , Clorpirifos/análise , Prata/química , Zircônio/química , Estruturas Metalorgânicas/química , Nanopartículas Metálicas/química , Espectrometria de Fluorescência , Limite de Detecção , Inseticidas/análise
10.
Int J Biol Macromol ; 278(Pt 1): 134637, 2024 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-39128734

RESUMO

Wounds are prone to infection which may be fatal to the life of the patient. The use of antibiotics is essential for managing bacterial infections in wounds, but the long-term use of high doses of antibiotics may lead to bacterial drug resistance and even to creation of superbacteria. Therefore, the development of targeted antimicrobial treatment strategies and the reduction in antibiotic usage are of utmost urgency. In this study, a multifunctional nanodrug delivery system (Cef-rhEGF@ZIF-8@ConA) for the treatment of bacteriostatic infection was synthesized through self-assembly of Zn2+, cefradine (Cef) and recombinant human epidermal growth factor (rhEGF), then conjugated with concanavalin (ConA), which undergoes pH-responsive degradation to release the drugs. First, ConA can specifically combine with bacteria and inhibit the rapid release of Zn2+ ions, thus achieving a long-acting antibacterial effect. Cef exerts its antibacterial effect by inhibiting the synthesis of bacterial membrane proteins. Finally, Zn2+ ions released from the Zn-metal-organic framework (MOF) demonstrate bacteriostatic properties by enhancing the permeability of the bacterial cell membrane. Furthermore, rhEGF upregulates angiogenesis-associated genes, thereby promoting angiogenesis, re-epithelialization and wound healing processes. The results showed that Cef-rhEGF@ZIF-8@ConA has good biocompatibility, with antibacterial efficacy against Staphylococcus aureus and Escherichia coli of 99.61 % and 99.75 %, respectively. These nanomaterials can inhibit the release of inflammatory cytokines and promote the release of anti-inflammatory cytokines, while also stimulating the proliferation of fibroblasts to facilitate wound healing. Taken together, the Cef-rhEGF@ZIF-8@ConA nanosystem is an excellent candidate in clinical therapeutics for bacteriostatic infection and wound healing.

11.
Small ; : e2405932, 2024 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-39171771

RESUMO

Semiconductive metal-organic frameworks (MOFs) with donor-acceptor (D-A) characteristics have garnered attractive attention due to their capacity for separating and transferring photogenerated charges, making them promising candidates for high-performance X-ray detectors. However, the low charge transfer efficiency between the metal nodes and organic ligands limits the X-ray-to-electricity conversion efficiency of these materials. Herein, an additional photoactive donor (D') is introduced by incorporating a heavy atom-containing polyoxometalate (POM) [α-SiW12O40]4- into a binary {[Ni·bcbp·(H2O)2]·(H2O)4·Cl}n (Ni-bcbp, bcbp: H2bcbp·2Cl = 1,1'-bis(4-carboxyphenyl)(4,4'-bipyridinium) dichloride) MOF, resulting in a semiconductive ternary D-D'-A framework {[Ni2(bcbp)2·(H2O)4·(DMA)]·(SiW12O40)}n (SiW@Ni-bcbp, DMA: dimethylacetamide). The obtained material features an unprecedented porous 8-connected bcu-net structure that accommodates nanoscale [α-SiW12O40]4- counterions, displaying uncommon optoelectronic responses. In contrast to binary Ni-bcbp, the SiW@Ni-bcbp framework exhibits distinctive photochromism and robust X-ray responsiveness, which can be attributed to the synergistic effects of the electron reservoir and multiple photoinduced electron transfer originating from the POMs. As a result, the X-ray detector based on SiW@Ni-bcbp demonstrates a sensitivity of 5741.6 µC Gyair -1 cm-2 with a low detection limit of 0.49 µGyair s-1. Moreover, the devices demonstrated the capability of producing clearness X-ray images, providing a feasible and stable solution for constructing high-performance direct X-ray detectors.

12.
J Chromatogr A ; 1733: 465259, 2024 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-39178659

RESUMO

Aluminum-based metal organic framework composite containing ionic liquid was prepared and used as sorbent for extraction of sixteen polycyclic aromatic hydrocarbons in list of priority pollutants of United States Environmental Protection Agency before their analysis by gas chromatography/mass spectrometry. The dispersive micro solid-phase extraction method, known as a simple and fast method, was preferred as the extraction method. The optimized parameter conditions were 5 mL of sample solution, 10 min sonication by ultrasonic bath, 30 mg of sorbent, 30 °C extraction temperature, 0.1 mL of hexane as elution solvent with 5 min elution time. The suggested method presented that limit of detection and limit of quantification were in the range of 0.01-0.10 µg l-1, and 0.04-0.33 µg L-1, respectively. The intra-day and inter-day repeatability were within the ranges of 1.18-4.88 % and 1.02-5.06 %, respectively. The recoveries for polycyclic aromatic hydrocarbons in peach juice, cherry juice, tap water and rain water samples were obtained in the range of 84.9-99.9 % for spiked 5, 50 and 100 µg l-1 standard polycyclic aromatic hydrocarbons solution.

13.
J Colloid Interface Sci ; 677(Pt B): 1022-1033, 2024 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-39178666

RESUMO

Transition metal-coordinated porphyrin metal-organic frameworks (MOFs) were perspective in photodynamic therapy (PDT) and catalytic therapy. However, the tumor hypoxia and the insufficient endogenous hydrogen peroxide (H2O2) seriously limited their efficacies. Herein, by encapsulating ultrasmall iridium (Ir) and modifying glucose oxidase (GOx), an iron-coordinated porphyrin MOF (Fe-MOF) nanoplatform (Fe-MOF@Ir/GOx) was designed to strengthen PDT/catalytic therapy by producing reactive oxygen species (ROS) storm. In this nanoplatform, Fe-MOF showed glutathione (GSH)-responsive degradation, by which porphyrin, GOx and ultrasmall Ir were released. Moreover, ultrasmall Ir possessed dual-activities of catalase (CAT)-like and peroxidase (POD)-like, which provided sufficient oxygen (O2) to enhance PDT efficacy, and hydroxyl radical (·OH) production was also improved by combining Fenton reaction of Fe2+. Further, GOx catalyzed endogenous glucose produced H2O2, also reduced pH value, which accelerated Fenton reaction and resulted in generation of ROS storm. Therefore, the developed Fe-MOF@Ir/GOx nanoplatform demonstrated enhanced PDT/catalytic therapy by producing ROS storm, and also provided a promising strategy to promote degradation/metabolism of inorganic nanoplatforms.

14.
Environ Res ; : 119825, 2024 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-39179142

RESUMO

In this study, we developed new adsorbents derived from orange peel biochar (BCOP) and enhanced them with CoFe2O4 magnetic nanoparticles (BCOP/CoFe2O4) and MIL-53(Al) (BCOP/CoFe2O4/MIL-53(Al)). These adsorbents were utilized to remove fluoride (FL) ions from aqueous solutions. We analyzed the properties of these adsorbents using a range of techniques, including FTIR, XRD, SEM, EDX-Map, VSM, Raman spectroscopy, and BET. Our findings indicate that the components interact effectively with one another. Specifically, the BCOP/CoFe2O4/MIL-53(Al) sample exhibited a specific surface area of 196.430 m2/g and a magnetic saturation value of 9.704 emu/g. The maximum FL ion adsorption capacities for BCOP, BCOP/CoFe2O4, and BCOP/CoFe2O4/MIL-53(Al) were 7.618, 16.330, and 37.320 mg/g, respectively, indicating that the modifications significantly enhanced the adsorption capacity. The optimum fluoride ion removal rates using BCOP, BCOP/CoFe2O4, and BCOP/CoFe2O4/MIL-53(Al) were 97.88%, 98.23%, and 99.06%, respectively, at adsorbent doses of 2.5, 1.5, and 0.8 g/L, contact times of 90, 70, and 50 minutes, pH 4, temperature 50°C, and a FL concentration of 10 mg/L. Thermodynamic studies revealed that the adsorption process was spontaneous and endothermic, with increased randomness between the adsorbent and fluoride ions. Kinetic analyses showed that fluoride ion adsorption by BCOP/CoFe2O4/MIL-53(Al) followed a pseudo-second-order (PSO) model, while BCOP and BCOP/CoFe2O4 followed a pseudo-first-order (PFO) model. Additionally, the equilibrium data for fluoride ion adsorption on BCOP/CoFe2O4/MIL-53(Al) adhered to the Freundlich model, whereas the other samples conformed to the Langmuir model. The study evaluates the effectiveness of BCOP, BCOP/CoFe2O4, and BCOP/CoFe2O4/MIL-53(Al) in removing FL ions from glass manufacturing wastewater, highlighting the superior performance of the magnetic composite due to its enhanced surface area and functional groups. Notably, the adsorbents demonstrated good regenerative capabilities, maintaining high performance over multiple adsorption cycles.

15.
Spectrochim Acta A Mol Biomol Spectrosc ; 323: 124898, 2024 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-39116597

RESUMO

Because ascorbic acid (AA) is one of the basic elements to maintain the normal physiological functions of human body, it is urgent to develop a material that can achieve efficient, rapid and in-situ detection for AA. A new fluorescence organic compound 4',4'''-(benzo[c][1,2,5]thiadiazole-4,7-diyl)bis([1,1'-biphenyl]-4-carboxylic acid) (H2BTBC) based on benzothiadiazole group has been synthesized, which can detect Fe3+ ions by fluorescence turn-off effect with a detection limit of 0.015 µM, as well as recognize linear amines by fluorescence turn-on effect. Moreover, a highly stable Tb(III) metal-organic framework has been solvothermally prepared with H2BTBC, namely {[(CH3)2NH2]2[Tb2(BTBC)4]∙solvents}n (JXUST-39), which can selectively detect AA among biological fluids by fluorescence enhancement effect with a detection limit of 0.077 µM. In addition, the mechanism for JXUST-39 detecting AA is possibly the cooperative effect of absorbance-caused enhancement and charge transfer between JXUST-39 and AA. Moreover, LED lamp beads, fluorescent films and fluorescent detection test paper based on JXUST-39 were prepared to achieve portable detection via fluorescence enhancement effect.

16.
Bioresour Technol ; 411: 131324, 2024 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-39179136

RESUMO

To achieve efficient dye degradation, we reported a visible light-driven biomass photo-enzyme coupled system, which was constructed by assembling g-C3N4 during in situ culture and immobilizing laccase via metal-organic framework (MOF). Benefited from the network and porous structure of bacterial cellulose (BC), the g-C3N4 could be stably interspersed, and MOF grew g-C3N4/BC to encapsulate laccase. BC improves the reusability of the system, while combined with MOF encapsulation, avoiding direct contact between photo- and enzyme- catalysts. Importantly, thanks to the existence of electron transfer from photocatalysis to enzyme, the photogenerated electron hole recombination within the photocatalyst reduced, improving catalyzed reaction efficiency. The degradation efficiency of the catalysis system within 10 min for methylene blue and rhodamine B could reach 100 % and 96.1 %, respectively, which could rapidly degrade dye and recycle for more than 10 times. This research can shine new light on the development of advanced wastewater treatment.

17.
Angew Chem Int Ed Engl ; : e202412340, 2024 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-39183598

RESUMO

Photocatalytic N2 reduction reaction (PNRR) offers a promising strategy for sustainable production of ammonia (NH3). However, the reported photocatalysts suffer from low efficiency with great room to improve regarding the charge carrier utilization and active site engineering. Herein, a porous and chemically bonded heterojunction photocatalyst is developed for efficient PNRR to NH3 production via hybridization of two semiconducting metal-organic frameworks (MOFs), MIL-125-NH2 (MIL=Material Institute Lavoisier) and Co-HHTP (HHTP=2,3,6,7,10,11-hexahydroxytripehenylene). Experimental and theoretical results demonstrate the formation of Ti-O-Co chemical bonds at the interface, which not only serve as atomic pathway for S-scheme charge transfer, but also provide electron-deficient Co centers for improving N2 chemisorption/activation capability and restricting competitive hydrogen evolution. Moreover, the nanoporous structure allows the transportation of reactants to the interfacial active sites at heterojunction, enabling the efficient utilization of charge carriers. Consequently, the rationally designed MOF-based heterojunction exhibits remarkable PNRR performance with an NH3 production rate of 2.1 mmol g-1 h-1, an apparent quantum yield (AQY) value of 16.2% at 365 nm and a solar-to-chemical conversion (SCC) efficiency of 0.28%, superior to most reported PNRR photocatalysts. Our work provides new insights into the design principles of high-performance photocatalysts.

18.
Adv Healthc Mater ; : e2402266, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39138999

RESUMO

Microwave (MW) therapy is an emerging therapy with high efficiency and deep penetration to combat the crisis of bacterial resistance. However, as the energy of MW is too low to induce electron transition, the mechanism of MW catalytic effect remains ambiguous. Herein, a cerium-based metal-organic framework (MOF) is fabricated and used in MW therapy. The MW-catalytic performance of CeTCPP is largely dependent on the ions in the liquid environment, and the electron transition is achieved through a "tribovoltaic effect" between water molecules and CeTCPP. By this way, CeTCPP can generate reactive oxygen species (ROS) in saline under pulsed MW irradiation, showing 99.9995 ± 0.0002% antibacterial ratio against Staphylococcus aureus (S. aureus) upon two cycles of MW irradiation. Bacterial metabolomics further demonstrates that the diffusion of ROS into bacteria led to the bacterial metabolic disorders. The bacteria are finally killed due to "amino acid starvation". In order to improve the applicability of CeTCPP, It is incorporated into alginate-based hydrogel, which maintains good MW catalytic antibacterial efficiency and also good biocompatibility. Therefore, this work provides a comprehensive instruction of using CeTCPP in MW therapy, from mechanism to application. This work also provides new perspectives for the design of antibacterial composite hydrogel.

19.
Talanta ; 280: 126535, 2024 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-39121618

RESUMO

Development of fresh solid phase extractant is critical for selective separation and purification of special proteins. Herein, we demonstrated a recombinant Staphylococcal Protein G (rSPG) with a His-tag modified the novel single-metal organic framework (rSPG@Ni-MOF-74). The proposed solid-phase extraction material possessed a uniform spindle-shaped structure, large surface area (709.60 m2 g-1) and pore volume (0.08 m3 g-1), high metal content (22.57 wt%), which facilitated the interaction between host and guest. As results, the composite displayed outstanding selective recognition and adsorption of IgG, due to synergistic effect of the binding ability of rSPG with the Fc region of IgG, maintained through hydrogen bonding and electrostatic attraction, as well as hydrophobic interaction. The adsorption performance and mechanism of rSPG@Ni-MOF-74 have been fully investigated. Additionally, the rSPG@Ni-MOF-74 composite could effectively separate IgG from serum obtained from healthy humans, with the purity of the separated IgG verified through SDS-PAGE analysis. Furthermore, LC-MS/MS analysis identified a high content of IgG (55.3 %) in the eluate from rSPG@Ni-MOF-74, suggesting the great potential of rSPG@Ni-MOF-74 in IgG separation and enrichment from complex matrix.

20.
Food Chem ; 460(Pt 3): 140774, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39121765

RESUMO

The development of a highly selective and sensitive method for detecting chlortetracycline (CTC) is crucial for safeguarding public health and food safety. Herein, a novel ratiometric fluorescence sensor called SiC@ZIF-8@MIP was constructed to specifically recognize and sensitively detect CTC. The sensor has the advantages of fast response speed (7 min), wide linear range (0.1-18 µg mL-1), and low limit of detection (4.56 ng mL-1). With the addition of CTC, the fluorescence of SiC@ZIF-8@MIP is quenched at 410 nm due to the internal filtration effect (IFE) and a new fluorescence signal is generated at 515 nm by CTC due to the aggregation induced emission effect (AIE). Additionally, for rapid on-site detection of CTC, a smartphone is applied to digitize fluorescence images of SiC@ZIF-8@MIP, helping individuals read and analyze the images. This detection method is a promising strategy for on-site assessments of food safety and public health safety.

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