RESUMO
Natural phosphatases featuring paired metal sites inspire various advanced nanozymes with phosphatase-like activity as alternatives in practical applications. Numerous efforts to create point defects show limited metal site pairs, further resulting in insufficient activity. However, it remains a grand challenge to accurately engineer abundant metal site pairs in nanozymes. Herein, we report a grain-boundary-rich ceria metallene nanozyme (GB-CeO2) with phosphatase-like activity. Grain boundaries acting as the line or interfacial defects can effectively increase the content of Ce4+/Ce3+ site pairs to 72.28%, achieving a 49.28-fold enhancement in activity. Furthermore, abundant grain boundaries optimize the band structure to assist the photoelectron transfer under irradiation, which further increases the content of metal site pairs to 88.96% and finally realizes a 114.39-fold enhanced activity over that of CeO2 without irradiation. Given the different inhibition effects of pesticides on catalysts with and without irradiation, GB-CeO2 was successfully applied to recognize mixed toxic pesticides.
Assuntos
Cério , Cério/química , Catálise , Monoéster Fosfórico Hidrolases/química , Monoéster Fosfórico Hidrolases/metabolismo , Nanoestruturas/química , Praguicidas/químicaRESUMO
Single-atom nanozymes (SANs) are considered to be ideal substitutes for natural enzymes due to their high atom utilization. This work reported a strategy to manipulate the second coordination shell of the Ce atom and reshape the carbon carrier to improve the oxidase-like activity of SANs. Internally, S atoms were symmetrically embedded into the second coordination layer to form a Ce-N4S2-C structure, which reduced the energy barrier for O2 reduction, promoted the electron transfer from the Ce atom to O atoms, and enhanced the interaction between the d orbital of the Ce atom and p orbital of O atoms. Externally, in situ polymerization of mussel-inspired polydopamine on the precursor helps capture metal sources and protects the 3D structure of the carrier during pyrolysis. On the other hand, polyethylene glycol (PEG) modulated the interface of the material to enhance water dispersion and mass transfer efficiency. As a proof of concept, the constructed PEG@P@Ce-N/S-C was applied to the multimodal assay of butyrylcholinesterase activity.
Assuntos
Cério , Cério/química , Polietilenoglicóis/química , Oxirredutases/química , Oxirredutases/metabolismo , Butirilcolinesterase/química , Butirilcolinesterase/metabolismo , Polímeros/química , Indóis/química , Oxigênio/química , OxirreduçãoRESUMO
Rectifying the aberrant microenvironment of a disease through maintenance of redox homeostasis has emerged as a promising perspective with significant therapeutic potential for Alzheimer's disease (AD). Herein, we design and construct a novel nanozyme-boosted MOF-CRISPR platform (CMOPKP), which can maintain redox homeostasis and rescue the impaired microenvironment of AD. By modifying the targeted peptides KLVFFAED, CMOPKP can traverse the blood-brain barrier and deliver the CRISPR activation system for precise activation of the Nrf2 signaling pathway and downstream redox proteins in regions characterized by oxidative stress, thereby reinstating neuronal antioxidant capacity and preserving redox homeostasis. Furthermore, cerium dioxide possessing catalase enzyme-like activity can synergistically alleviate oxidative stress. Further in vivo studies demonstrate that CMOPKP can effectively alleviate cognitive impairment in 3xTg-AD mouse models. Therefore, our design presents an effective way for regulating redox homeostasis in AD, which shows promise as a therapeutic strategy for mitigating oxidative stress in AD.
Assuntos
Doença de Alzheimer , Estresse Oxidativo , Doença de Alzheimer/tratamento farmacológico , Doença de Alzheimer/metabolismo , Doença de Alzheimer/genética , Animais , Camundongos , Estresse Oxidativo/efeitos dos fármacos , Humanos , Fator 2 Relacionado a NF-E2/metabolismo , Estruturas Metalorgânicas/química , Modelos Animais de Doenças , Sistemas CRISPR-Cas/genética , Cério/química , Cério/uso terapêutico , Cério/farmacologia , Barreira Hematoencefálica/metabolismo , Oxirredução , Antioxidantes/química , Antioxidantes/farmacologia , Antioxidantes/uso terapêuticoRESUMO
In this work, a novel isatin-Schiff base L2 had been synthesized through a simple reaction between isatin and 2-amino-5-methylthio-1,3,4-thiadiazole. The produced Schiff base L2 was then subjected to a hydrothermal reaction with cerium chloride to produce the cerium (III)-Schiff base complex C2. Several spectroscopic methods, including mass spectra, FT-IR, elemental analysis, UV-vis, 13C-NMR, 1H-NMR, Thermogravimetric Analysis, HR-TEM, and FE-SEM/EDX, were used to completely characterize the produced L2 and C2. A computer simulation was performed using the MOE software program to find out the probable biological resistance of studied compounds against the proteins in some types of bacteria or fungi. To investigate the interaction between the ligand and its complex, we conducted molecular docking simulations using the molecular operating environment (MOE). The docking simulation findings revealed that the complex displayed greater efficacy and demonstrated a stronger affinity for Avr2 effector protein from the fungal plant pathogen Fusarium oxysporum (code 5OD4) than the original ligand. The antibacterial activity of the ligand and its Ce3+ complex were applied in vitro tests against different microorganism. The study showed that the complex was found to be more effective than the ligand.
Assuntos
Cério , Isatina , Simulação de Acoplamento Molecular , Espectroscopia de Infravermelho com Transformada de Fourier , Isatina/farmacologia , Isatina/química , Cério/farmacologia , Bases de Schiff/farmacologia , Bases de Schiff/química , Simulação por Computador , Ligantes , Antibacterianos/farmacologia , Testes de Sensibilidade MicrobianaRESUMO
The enhancement of sensitivity in biological analysis detection can reduce the probability of false positives of the biosensor. In this work, a novel self-on controlled-release electrochemiluminescence (CRE) biosensor was designed by multiple signal amplification and framework-enhanced stability strategies. As a result, the changes of the ECL signal were enhanced before and after the controlled-release process, achieving sensitive detection of prostate-specific antigen (PSA). Specifically, for one thing, Fe3O4@CeO2-NH2 with two paths for enhancing the generation of coreactant radicals was used as the coreaction accelerator to boost ECL performance. For another, due to the framework stability, zeolitic imidazolate framework-8-NH2 (ZIF-8-NH2) was combined with luminol to make the ECL signal more stable. Based on these strategies, the constructed CRE biosensor showed a strong self-on effect in the presence of PSA and high sensitivity in a series of tests. The detection range and limit of detection (LOD) were 5 fg/mL to 10 ng/mL and 2.8 fg/mL (S/N = 3), respectively, providing a feasible approach for clinical detection of PSA.
Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Medições Luminescentes , Antígeno Prostático Específico , Antígeno Prostático Específico/análise , Antígeno Prostático Específico/sangue , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Humanos , Limite de Detecção , Masculino , Cério/química , Luminol/químicaRESUMO
New strategies for the simultaneous and portable detection of multiple enzyme activities are highly desirable for clinical diagnosis and home care. However, the methods developed thus far generally suffer from high costs, cumbersome procedures, and heavy reliance on large-scale instruments. To satisfy the actual requirements of rapid, accurate, and on-site detection of multiple enzyme activities, we report herein a smartphone-assisted programmable microfluidic paper-based analytical device (µPAD) that utilizes colorimetric and photothermal signals for simultaneous, accurate, and visual quantitative detection of alkaline phosphatase (ALP) and butyrylcholinesterase (BChE). Specifically, the operation of this µPAD sensing platform is based on two sequential steps. Cobalt-doped mesoporous cerium oxide (Co-m-CeO2) with remarkable peroxidase-like activities under neutral conditions first catalytically decomposes H2O2 for effectively converting colorless 3,3',5,5'-tetramethylbenzidine (TMB) into blue oxidized TMB (oxTMB). The subsequent addition of ALP or BChE to their respective substrates produces a reducing substance that can somewhat inhibit the oxTMB transformation for compromised colorimetric and photothermal signals of oxTMB. Notably, these two-step bioenzyme-nanozyme cascade reactions strongly support the straightforward and excellent processability of this platform, which exhibit lower detection limits for ALP and BChE with a detection limit for BChE an order of magnitude lower than those of the other reported paper-based detection methods. The practicability and efficiency of this platform are further demonstrated through the analysis of clinical serum samples. This innovative platform exhibits great potential as a facile yet robust approach for simultaneous, accurate, and on-site visual detection of multiple enzyme activities in authentic samples.
Assuntos
Fosfatase Alcalina , Butirilcolinesterase , Colorimetria , Papel , Fosfatase Alcalina/metabolismo , Fosfatase Alcalina/análise , Fosfatase Alcalina/química , Humanos , Butirilcolinesterase/metabolismo , Butirilcolinesterase/sangue , Dispositivos Lab-On-A-Chip , Benzidinas/química , Smartphone , Cério/química , Cobalto/química , Técnicas Analíticas Microfluídicas/instrumentação , Limite de Detecção , Ensaios Enzimáticos/métodos , Ensaios Enzimáticos/instrumentação , Peróxido de Hidrogênio/química , Peróxido de Hidrogênio/análiseRESUMO
In this work, a microfluidic immunosensor chip was developed by incorporating microfluidic technology with electrochemiluminescence (ECL) for sensitive detection of human epidermal growth factor receptor-2 (HER2). The immunosensor chip can achieve robust reproducibility in mass production by integrating multiple detection units in a series. Notably, nanoscale materials can be better adapted to microfluidic systems, greatly enhancing the accuracy of the immunosensor chip. Ag@Au NCs closed by glutathione (GSH) were introduced in the ECL microfluidic immunosensor system with excellent and stable ECL performance. The synthesized CeO2-Au was applied as a coreaction promoter in the ECL signal amplification system, which made the result of HER2 detection more reliable. In addition, the designed microfluidic immunosensor chip integrated the biosensing system into a microchip, realizing rapid and accurate detection of HER2 by its high throughput and low usage. The developed short peptide ligand NARKFKG (NRK) achieved an effective connection between the antibody and nanocarrier for improving the detection efficiency of the sensor. The immunosensor chip had better storage stability and sensitivity than traditional detection methods, with a wide detection range from 10 fg·mL-1 to 100 ng·mL-1 and a low detection limit (LOD) of 3.29 fg·mL-1. In general, a microfluidic immunosensor platform was successfully constructed, providing a new idea for breast cancer (BC) clinical detection.
Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Eletrodos , Ouro , Medições Luminescentes , Nanopartículas Metálicas , Receptor ErbB-2 , Prata , Humanos , Receptor ErbB-2/análise , Receptor ErbB-2/imunologia , Nanopartículas Metálicas/química , Técnicas Eletroquímicas/métodos , Prata/química , Técnicas Biossensoriais/métodos , Ouro/química , Imunoensaio/métodos , Técnicas Analíticas Microfluídicas/instrumentação , Limite de Detecção , Cério/químicaRESUMO
The establishment of an osseointegration is crucial for the long-term stability and functionality of implant materials, and early angiogenesis is the key to successful osseointegration. However, the bioinertness of titanium implants affects osseointegration, limiting their clinical application. In this study, inspired by the rapid polarization of macrophages following the phagocytosis of bacteria, we developed bacteroid cerium oxide particles; these particles were composed of CeO2 and had a size similar to that of Bacillus (0.5 µ m). These particles were constructed on the implant surfaces using a hydrothermal method. In vitro experiments demonstrated that the particles effectively decreased the reactive oxygen species (ROS) levels in macrophages (RAW264.7). Furthermore, these particles exerted effects on M1 macrophage polarization, enhanced nitric oxide (NO) secretion to promote vascular regeneration, and facilitated rapid macrophage transition to the M2 phenotype. Subsequently, the particles facilitated human umbilical vein endothelial cell (HUVEC) migration. In vivo studies showed that these particles rapidly stimulated innate immune responses in animal models, leading to enhanced angiogenesis around the implant and improved osseointegration. In summary, the presence of bacteroid cerium oxide particles on the implant surface regulated and accelerated macrophage polarization, thereby enhancing angiogenesis during the immune response and improving peri-implant osseointegration.
Assuntos
Cério , Osseointegração , Animais , Humanos , Macrófagos , Cério/farmacologia , Imunidade Inata , Neovascularização Patológica , Titânio , Osteogênese , Propriedades de SuperfícieRESUMO
CeO2, particularly in the shape of rod, has recently gained considerable attention for its ability to mimic peroxidase (POD) and haloperoxidase (HPO). However, this multi-enzyme activities unavoidably compete for H2O2 affecting its performance in relevant applications. The lack of consensus on facet distribution in rod-shaped CeO2 further complicates the establishment of structure-activity correlations, presenting challenges for progress in the field. In this study, the HPO-like activity of rod-shaped CeO2 is successfully enhanced while maintaining its POD-like activity through a facile post-calcination method. By studying the spatial distribution of these two activities and their exclusive H2O2 activation pathways on CeO2 surfaces, this study finds that the increased HPO-like activity originated from the newly exposed (111) surface at the tip of the shortened rods after calcination, while the unchanged POD-like activity is attributed to the retained (110) surface in their lateral area. These findings not only address facet distribution discrepancies commonly reported in the literature for rod-shaped CeO2 but also offer a simple approach to enhance its antibacterial performance. This work is expected to provide atomic insights into catalytic correlations and guide the design of nanozymes with improved activity and reaction specificity.
Assuntos
Cério , Peróxido de Hidrogênio , Cério/química , Peróxido de Hidrogênio/metabolismo , Peróxido de Hidrogênio/química , Peroxidase/metabolismo , Peroxidase/químicaRESUMO
The improper use and overuse of antibiotics have led to significant burdens and detrimental effects on the environment, food supply, and human health. Herein, a magnetic solid-phase extraction program and an optical immunosensor based on bimetallic Ce/Zr-UiO 66 for the detection of antibiotics are developed. A magnetic Fe3O4@SiO2@Ce/Zr-UiO 66 metal-organic framework (MOF) is prepared to extract and enrich chloramphenicol from fish, wastewater, and urine samples, and a horseradish peroxidase (HRP)-Ce/Zr-UiO 66@bovine serum protein-chloramphenicol probe is used for the sensitive detection of chloramphenicol based on the dual-effect catalysis of Ce and HRP. In this manner, the application of Ce/Zr-UiO 66 in integrating sample pretreatment and antibiotic detection is systematically investigated and the associated mechanisms are explored. It is concluded that Ce/Zr-UiO 66 is a versatile dual-track material exhibiting high enrichment efficiency (6.37 mg g-1) and high sensitivity (limit of detection of 51.3 pg mL-1) for chloramphenicol detection and serving as a multifunctional MOF for safeguarding public health and hygiene.
Assuntos
Antibacterianos , Cloranfenicol , Estruturas Metalorgânicas , Estruturas Metalorgânicas/química , Cloranfenicol/análise , Animais , Humanos , Dióxido de Silício/química , Cério/química , Peroxidase do Rábano Silvestre/química , Peroxidase do Rábano Silvestre/metabolismoRESUMO
Doxorubicin (DOX) is an important drug for cancer treatment, but its clinical application is limited due to its toxicity and side effects. Therefore, detecting the concentration of DOX during treatment is crucial for enhancing efficacy and reducing side effects. In this study, the authors developed a biophotonic fiber sensor based on localized surface plasmon resonance (LSPR) with the multimode fiber (MMF)-four core fiber (FCF)-seven core fiber (SCF)-MMF-based direct-taper and anti-taper structures for the specific detection of DOX. Compared to other detection methods, it has the advantages of high sensitivity, low cost, and strong anti-interference ability. In this experiment, multi-walled carbon nanotubes (MWCNTs), cerium-oxide nanorods (CeO2-NRs), and gold nanoparticles (AuNPs) were immobilized on the probe surface to enhance the sensor's biocompatibility. MWCNTs and CeO2-NRs provided more binding sites for the fixation of AuNPs. By immobilizing AuNPs on the surface, the LSPR was stimulated by the evanescent field to detect DOX. The sensor surface was functionalized with DOX aptamers for specific detection, enhancing its specificity. The experiments demonstrated that within a linear detection range of 0-10 µM, the sensitivity of the sensor is 0.77 nm/µM, and the limit of detection (LoD) is 0.42 µM. Additionally, the probe's repeatability, reproducibility, stability, and selectivity were evaluated, indicating that the probe has high potential for detecting DOX during cancer treatment.
Assuntos
Doxorrubicina , Ouro , Nanopartículas Metálicas , Ressonância de Plasmônio de Superfície , Doxorrubicina/farmacologia , Humanos , Ressonância de Plasmônio de Superfície/instrumentação , Ouro/química , Nanopartículas Metálicas/química , Neoplasias/tratamento farmacológico , Nanotubos de Carbono/química , Técnicas Biossensoriais/instrumentação , Fibras Ópticas , Desenho de Equipamento , Antibióticos Antineoplásicos/análise , Cério/química , Tecnologia de Fibra Óptica/instrumentaçãoRESUMO
Ascorbic acid (AA), a prominent antioxidant commonly found in human blood serum, serves as a biomarker for assessing oxidative stress levels. Therefore, precise detection of AA is crucial for swiftly diagnosing conditions arising from abnormal AA levels. Consequently, the primary aim of this research is to develop a sensitive and selective electrochemical sensor for accurate AA determination. To accomplish this aim, we used a novel nanocomposite comprised of CeO2-doped ZnO adorned on biomass-derived carbon (CeO2·ZnO@BC) as the active nanomaterial, effectively fabricating a glassy carbon electrode (GCE). Various analytical techniques were employed to scrutinize the structure and morphology features of the CeO2·ZnO@BC nanocomposite, ensuring its suitability as the sensing nanomaterial. This innovative sensor is capable of quantifying a wide range of AA concentrations, spanning from 0.5 to 1925 µM in a neutral phosphate buffer solution. It exhibits a remarkable sensitivity of 0.2267 µA µM-1cm-2 and a practical detection limit of 0.022 µM. Thanks to its exceptional sensitivity and selectivity, this sensor enables highly accurate determination of AA concentrations in real samples. Moreover, its superior reproducibility, repeatability, and stability underscore its reliability and robustness for AA quantification.
Assuntos
Ácido Ascórbico , Carbono , Cério , Técnicas Eletroquímicas , Nanocompostos , Óxido de Zinco , Ácido Ascórbico/análise , Ácido Ascórbico/química , Ácido Ascórbico/sangue , Nanocompostos/química , Óxido de Zinco/química , Técnicas Eletroquímicas/métodos , Cério/química , Carbono/química , Humanos , Biomassa , Eletrodos , Limite de DetecçãoRESUMO
The presence of oxidative stress in bone defects leads to delayed regeneration, especially in the aged population and patients receiving cancer treatment. This delay is attributed to the increased levels of reactive oxygen species (ROS) in these populations due to the accumulation of senescent cells. Tissue-engineered scaffolds are emerging as an alternative method to treat bone defects. In this study, we engineered tissue scaffolds tailored to modulate the adverse effects of oxidative stress and promote bone regeneration. We used polycaprolactone to fabricate nanofibrous mats by using electrospinning. We exploited the ROS-scavenging properties of cerium oxide nanoparticles to alleviate the high oxidative stress microenvironment caused by the presence of senescent cells. We characterized the nanofibers for their physical and mechanical properties and utilized an ionization-radiation-based model to induce senescence in bone cells. We demonstrate that the presence of ceria can modulate ROS levels, thereby reducing the level of senescence and promoting osteogenesis. Overall, this study demonstrates that ceria-infused nanofibrous scaffolds can be used for augmenting the osteogenic activity of senescent progenitor cells, which has important implications for engineering bone tissue scaffolds for patients with low regeneration capabilities.
Assuntos
Regeneração Óssea , Senescência Celular , Cério , Nanofibras , Osteogênese , Espécies Reativas de Oxigênio , Engenharia Tecidual , Alicerces Teciduais , Cério/química , Cério/farmacologia , Regeneração Óssea/efeitos dos fármacos , Alicerces Teciduais/química , Senescência Celular/efeitos dos fármacos , Nanofibras/química , Osteogênese/efeitos dos fármacos , Humanos , Engenharia Tecidual/métodos , Espécies Reativas de Oxigênio/metabolismo , Estresse Oxidativo/efeitos dos fármacos , Poliésteres/química , Animais , Osso e Ossos/efeitos dos fármacosRESUMO
BACKGROUND: Spinal cord injury (SCI) remained one of the challenges to treat due to its complicated mechanisms. Photobiomodulation therapy (PBMT) accelerates neuronal regeneration. Cerium oxide nanoparticles (CeONPs) also eliminate free radicals in the environment. The present study aims to introduce a combined treatment method of making PCL scaffolds as microenvironments, seeded with CeONPs and the PBMT technique for SCI treatment. METHODS: The surgical hemi-section was used to induce SCI. Immediately after the SCI induction, the scaffold (Sc) was loaded with CeONPs implanted. PBMT began 30 min after SCI induction and lasted for up to 4 weeks. Fifty-six male rats were randomly divided into seven groups. Glial fibrillary acidic protein (GFAP) (an astrocyte marker), Connexin 43 (Con43) (a member of the gap junction), and gap junctions (GJ) (a marker for the transfer of ions and small molecules) expressions were evaluated. The behavioral evaluation was performed by BBB, Acetone, Von Frey, and radiant heat tests. RESULT: The SC + Nano + PBMT group exhibited the most remarkable recovery outcomes. Thermal hyperalgesia responses were mitigated, with the combined approach displaying the most effective relief. Mechanical allodynia and cold allodynia responses were also attenuated by treatments, demonstrating potential pain management benefits. CONCLUSION: These findings highlight the potential of PBMT, combined with CeONPs-loaded scaffolds, in promoting functional motor recovery and alleviating pain-related responses following SCI. The study underscores the intricate interplay between various interventions and their cumulative effects, informing future research directions for enhancing neural repair and pain management strategies in SCI contexts.
Assuntos
Cério , Terapia com Luz de Baixa Intensidade , Traumatismos da Medula Espinal , Ratos , Masculino , Animais , Terapia com Luz de Baixa Intensidade/efeitos adversos , Dor/complicações , Traumatismos da Medula Espinal/radioterapia , Traumatismos da Medula Espinal/complicações , HiperalgesiaRESUMO
One of the crucial metabolic processes for both plant and animal kingdoms is the oxidation of the amino acid tryptophan (TRP) that regulates plant growth and controls hunger and sleeping patterns in animals. Here, we report revolutionary insights into how this process can be crucially affected by interactions with metal oxide nanoparticles (NPs), creating a toolbox for a plethora of important biomedical and agricultural applications. Molecular mechanisms in TRP-NP interactions were revealed by NMR and optical spectroscopy for ceria and titania and by X-ray single-crystal study and a computational study of model TRP-polyoxometalate complexes, which permitted the visualization of the oxidation mechanism at an atomic level. Nanozyme activity, involving concerted proton and electron transfer to the NP surface for oxides with a high oxidative potential, like CeO2 or WO3, converted TRP in the first step into a tricyclic organic acid belonging to the family of natural plant hormones, auxins. TiO2, a much poorer oxidant, was strongly binding TRP without concurrent oxidation in the dark but oxidized it nonspecifically via the release of reactive oxygen species (ROS) in daylight.
Assuntos
Nanopartículas Metálicas , Triptofano , Cério/química , Nanopartículas Metálicas/química , Modelos Moleculares , Oxirredução , Óxidos/química , Titânio/química , Triptofano/química , Triptofano/metabolismoRESUMO
The removal of pollutants from water bodies is crucial for the well-being of humanity and is a topic of global research. Researchers have turned their attention to green synthesized nanoparticles for wastewater treatment due to their eco-friendly nature, biocompatibility, and cost-effectiveness. This work demonstrates the efficient removal of organic dye and both gram-positive and gram-negative bacteria from water bodies using copper-doped cerium oxide nanoparticles synthesized withMurraya Koenigiiextract. Characterized via various methods, the 15% copper doped cerium oxide nanoparticles (Cu 15% NPs) exhibited maximum Congo red dye adsorption (98% degradation in 35 min). Kinetic analysis favoured a pseudo-second-order model, indicating the chemical nature of adsorption. Equilibrium adsorption isotherms aligned with the Langmuir model, indicating homogenous monolayer dye adsorption on the doped adsorbent. The maximum uptake of adsorbate,Qmobtained from Langmuir model for Cu 15% NPs was 193 mg g-1. The study also showed enhanced antibacterial activity againstBacillus subtilis, Staphylococcus aureus, Escherichia coliandPseudomonas aeruginosafor Cu-doped ceria, attributed to generation of reactive oxygen species (ROS) induced by the redox cycling between Ce3+and Ce4+. This substantiated that the green synthesized copper doped cerium oxide nanoparticles are potential candidates for adsorptive removal of Congo red dye and as antibacterial agents.
Assuntos
Cério , Nanopartículas Metálicas , Poluentes Químicos da Água , Vermelho Congo , Cobre/química , Adsorção , Cinética , Antibacterianos/farmacologia , Antibacterianos/química , Bactérias Gram-Negativas , Bactérias Gram-Positivas , Nanopartículas Metálicas/química , Água/química , Concentração de Íons de HidrogênioRESUMO
It is a promising research direction to develop catalysts with high stability and ozone utilization for low-temperature ozone catalytic oxidation of VOCs. While bimetallic catalysts exhibit excellent catalytic activity compared with conventional single noble metal catalysts, limited success has been achieved in the influence of the bimetallic effect on the stability and ozone utilization of metal catalysts. Herein, it is necessary to systematically study the enhancement effect in the ozone catalytic reaction induced by the second metal. With a simple continuous impregnation method, a platinum-cerium bimetallic catalyst is prepared. Also highlighted are studies from several aspects of the contribution of the second metal (Ce) to the stability and ozone utilization of the catalysts, including the "electronic effect" and "geometric effect". The synergistic removal rate of toluene and ozone is nearly 100% at 30 °C, and it still shows positive stability after high humidity and a long reaction time. More importantly, the instructive significance, which is the in-depth knowledge of enhanced catalytic mechanism of bimetallic catalysts resulting from a second metal, is provided by this work.
Assuntos
Cério , Ozônio , Oxirredução , Metais , CatáliseRESUMO
Environmentally benign cerium-based catalysts are promising alternatives to toxic vanadium-based catalysts for controlling NOx emissions via selective catalytic reduction (SCR), but conventional cerium-based catalysts unavoidably suffer from SO2 poisoning in low-temperature SCR. We develop a strongly sulfur-resistant Ce1+1/TiO2 catalyst by spatially confining Ce atom pairs to different anchoring sites of anatase TiO2(001) surfaces. Experimental results combined with theoretical calculations demonstrate that strong electronic interactions between the paired Ce atoms upshift the lowest unoccupied states to an energy level higher than the highest occupied molecular orbital (HOMO) of SO2 so as to be catalytically inert in SO2 oxidation but slightly lower than HOMO of NH3 so that Ce1+1/TiO2 has desired ability toward NH3 activation required for SCR. Hence, Ce1+1/TiO2 shows higher SCR activity and excellent stability in the presence of SO2 at low temperatures with respect to supported single Ce atoms. This work provides a general strategy to develop sulfur-resistant catalysts by tuning the electronic states of active sites for low-temperature SCR, which has implications for practical applications with energy-saving requirements.
Assuntos
Cério , Enxofre , Cério/química , Enxofre/química , Catálise , Oxirredução , TemperaturaRESUMO
Investigating the ternary relationship among nanoparticles (NPs), their immediate molecular environment, and test organisms rather than the direct interaction between pristine NPs and test organisms has been thrust into the mainstream of nanotoxicological research. Diverging from previous work that predominantly centered on surrounding molecules affecting the toxicity of NPs by modulating their nanoproperties, this study has unveiled a novel dimension: surrounding molecules altering bacterial susceptibility to NPs, consequently impacting the outcomes of nanobio interaction. The study found that adding nitrate as the surrounding molecules could alter bacterial respiratory pathways, resulting in an enhanced reduction of ceria NPs (nanoceria) on the bacterial surfaces. This, in turn, increased the ion-specific toxicity originating from the release of Ce3+ ions at the nanobio interface. Further transcriptome analysis revealed more mechanistic details underlying the nitrate-induced changes in the bacterial energy metabolism and subsequent toxicity patterns. These findings offer a new perspective for the deconstruction of nanobio interactions and contribute to a more comprehensive understanding of NPs' environmental fate and ecotoxicity.
Assuntos
Cério , Cério/toxicidade , Cério/química , Bactérias/metabolismo , Nanopartículas/toxicidade , Nanopartículas Metálicas/toxicidade , Nanopartículas Metálicas/químicaRESUMO
The excessive energy consumed restricts the application of traditional postcombustion CO2 capture technology and limits the achievement of carbon-neutrality goals. Catalytic-rich CO2 amine regeneration has the potential to accelerate proton transfer and increase the energy efficiency in the CO2 separation process. Herein, we reported a Ce-metal-organic framework (MOF)-derived composite catalyst named HZ-Ni@UiO-66 with a hierarchical structure, which can increase the CO2 desorbed amount by 57.7% and decrease the relative heat duty by 36.5% in comparison with the noncatalytic monoethanolamine (MEA) regeneration process. The composite catalyst of the CeO2 coating from the UiO-66 precursor on the HZ-Ni carrier shows excellent stability with a long lifespan. The HZ-Ni@UiO-66 catalyst also shows a universal catalytic effect in typical blended amine systems with a large cyclic capacity. The HZ-Ni@UiO-66 catalyst effectively decreases the energy barrier of the CO2 desorption reaction to reduce the time required to reach thermodynamics, consequently saving the energy consumption generated by water evaporation. This research provides a new avenue for advancing amine regeneration with less heat duty at low temperatures.