Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 59
Filtrar
Más filtros










Base de datos
Intervalo de año de publicación
1.
Nat Commun ; 15(1): 3356, 2024 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-38637502

RESUMEN

To realize economically feasible electrochemical CO2 conversion, achieving a high partial current density for value-added products is particularly vital. However, acceleration of the hydrogen evolution reaction due to cathode flooding in a high-current-density region makes this challenging. Herein, we find that partially ligand-derived Ag nanoparticles (Ag-NPs) could prevent electrolyte flooding while maintaining catalytic activity for CO2 electroreduction. This results in a high Faradaic efficiency for CO (>90%) and high partial current density (298.39 mA cm‒2), even under harsh stability test conditions (3.4 V). The suppressed splitting/detachment of Ag particles, due to the lipid ligand, enhance the uniform hydrophobicity retention of the Ag-NP electrode at high cathodic overpotentials and prevent flooding and current fluctuations. The mass transfer of gaseous CO2 is maintained in the catalytic region of several hundred nanometers, with the smooth formation of a triple phase boundary, which facilitate the occurrence of CO2RR instead of HER. We analyze catalyst degradation and cathode flooding during CO2 electrolysis through identical-location transmission electron microscopy and operando synchrotron-based X-ray computed tomography. This study develops an efficient strategy for designing active and durable electrocatalysts for CO2 electrolysis.

2.
EMBO Mol Med ; 16(3): 506-522, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38374465

RESUMEN

Fragile X syndrome (FXS) is the leading cause of inherited autism and intellectual disabilities. Aberrant protein synthesis due to the loss of fragile X messenger ribonucleoprotein (FMRP) is the major defect in FXS, leading to a plethora of cellular and behavioral abnormalities. However, no treatments are available to date. In this study, we found that activation of metabotropic glutamate receptor 7 (mGluR7) using a positive allosteric modulator named AMN082 represses protein synthesis through ERK1/2 and eIF4E signaling in an FMRP-independent manner. We further demonstrated that treatment of AMN082 leads to a reduction in neuronal excitability, which in turn ameliorates audiogenic seizure susceptibility in Fmr1 KO mice, the FXS mouse model. When evaluating the animals' behavior, we showed that treatment of AMN082 reduces repetitive behavior and improves learning and memory in Fmr1 KO mice. This study uncovers novel functions of mGluR7 and AMN082 and suggests the activation of mGluR7 as a potential therapeutic approach for treating FXS.


Asunto(s)
Compuestos de Bencidrilo , Síndrome del Cromosoma X Frágil , Receptores de Glutamato Metabotrópico , Ratones , Animales , Proteína de la Discapacidad Intelectual del Síndrome del Cromosoma X Frágil/genética , Proteína de la Discapacidad Intelectual del Síndrome del Cromosoma X Frágil/metabolismo , Síndrome del Cromosoma X Frágil/tratamiento farmacológico , Síndrome del Cromosoma X Frágil/genética , Receptores de Glutamato Metabotrópico/metabolismo , Modelos Animales de Enfermedad , Ratones Noqueados
3.
EMBO Rep ; 25(3): 1233-1255, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38413732

RESUMEN

Accumulation of amyloid-beta (Aß) can lead to the formation of aggregates that contribute to neurodegeneration in Alzheimer's disease (AD). Despite globally reduced neural activity during AD onset, recent studies have suggested that Aß induces hyperexcitability and seizure-like activity during the early stages of the disease that ultimately exacerbate cognitive decline. However, the underlying mechanism is unknown. Here, we reveal an Aß-induced elevation of postsynaptic density protein 95 (PSD-95) in cultured neurons in vitro and in an in vivo AD model using APP/PS1 mice at 8 weeks of age. Elevation of PSD-95 occurs as a result of reduced ubiquitination caused by Akt-dependent phosphorylation of E3 ubiquitin ligase murine-double-minute 2 (Mdm2). The elevation of PSD-95 is consistent with the facilitation of excitatory synapses and the surface expression of α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid (AMPA) receptors induced by Aß. Inhibition of PSD-95 corrects these Aß-induced synaptic defects and reduces seizure activity in APP/PS1 mice. Our results demonstrate a mechanism underlying elevated seizure activity during early-stage Aß pathology and suggest that PSD-95 could be an early biomarker and novel therapeutic target for AD.


Asunto(s)
Enfermedad de Alzheimer , Precursor de Proteína beta-Amiloide , Animales , Ratones , Enfermedad de Alzheimer/metabolismo , Péptidos beta-Amiloides/metabolismo , Precursor de Proteína beta-Amiloide/metabolismo , Modelos Animales de Enfermedad , Ratones Transgénicos , Densidad Postsináptica/metabolismo , Densidad Postsináptica/patología , Receptores AMPA/metabolismo , Convulsiones
4.
Mol Psychiatry ; 28(9): 3782-3794, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37759036

RESUMEN

Synaptic potentiation underlies various forms of behavior and depends on modulation by multiple activity-dependent transcription factors to coordinate the expression of genes necessary for sustaining synaptic transmission. Our current study identified the tumor suppressor p53 as a novel transcription factor involved in this process. We first revealed that p53 could be elevated upon chemically induced long-term potentiation (cLTP) in cultured primary neurons. By knocking down p53 in neurons, we further showed that p53 is required for cLTP-induced elevation of surface GluA1 and GluA2 subunits of α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid receptor (AMPAR). Because LTP is one of the principal plasticity mechanisms underlying behaviors, we employed forebrain-specific knockdown of p53 to evaluate the role of p53 in behavior. Our results showed that, while knocking down p53 in mice does not alter locomotion or anxiety-like behavior, it significantly promotes repetitive behavior and reduces sociability in mice of both sexes. In addition, knocking down p53 also impairs hippocampal LTP and hippocampus-dependent learning and memory. Most importantly, these learning-associated defects are more pronounced in male mice than in female mice, suggesting a sex-specific role of p53 in these behaviors. Using RNA sequencing (RNAseq) to identify p53-associated genes in the hippocampus, we showed that knocking down p53 up- or down-regulates multiple genes with known functions in synaptic plasticity and neurodevelopment. Altogether, our study suggests p53 as an activity-dependent transcription factor that mediates the surface expression of AMPAR, permits hippocampal synaptic plasticity, represses autism-like behavior, and promotes hippocampus-dependent learning and memory.


Asunto(s)
Trastorno Autístico , Animales , Femenino , Masculino , Ratones , Trastorno Autístico/metabolismo , Hipocampo/metabolismo , Potenciación a Largo Plazo/fisiología , Plasticidad Neuronal/genética , Receptores AMPA/genética , Receptores AMPA/metabolismo , Sinapsis/metabolismo , Factores de Transcripción/metabolismo , Proteína p53 Supresora de Tumor/genética , Proteína p53 Supresora de Tumor/metabolismo
5.
Sci Total Environ ; 893: 164892, 2023 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-37327901

RESUMEN

In urban areas, particulate matter emitted from vehicles directly affects the health of citizens near roads. Thus, in this study, particle size distribution was measured by the horizontal and vertical distances along a highway road with heavy traffic to characterize the dispersion phenomena of particulate matter emitted from vehicles. In addition, the contribution of pollution sources was analyzed using a source-receptor model. A concentration gradient was observed in which the concentration decreased with the increase in the distance from the road when the wind blew from the road to the monitoring locations. The concentration was slightly higher within 50 m of the road when the wind blows parallel to the road, and similar concentrations were found at the other monitoring locations further away from the roads. In particular, the higher the turbulence intensity of the wind, the lower is the concentration gradient coefficient because of the more enhanced mixing and dispersion. A positive matrix factorization (PMF) model with the measured particle size distribution data in the range of 9-300 nm resulted in a contribution of about 70 % (number) and 20 % (mass) to particle concentrations because of six types of vehicles including LPG, two gasoline vehicles (GDI, MPI), and three diesel vehicles with 3rd, 4th, and 5th emission classes. It showed a decrease in the vehicular contribution as the distance from the road increased. Particle number concentrations decreased with increasing altitude up to 30 m above the ground. The results of this study can be useful in deriving generalized gradient equations of particle concentrations exposed by distance and wind direction at the roadside using traffic and meteorological conditions and for establishing environmental policies, such as roadside exposure assessment, in the future. A CAPSULE ABSTRACT: Dispersion of particles emitted from vehicles on a busy highway was characterized by roadside measurements of horizontal and vertical profiles of particle size distributions measured at four locations. The source profiles and contributions were estimated by major sources using a source-receptor model such as PMF.

6.
ChemSusChem ; 15(10): e202200375, 2022 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-35293137

RESUMEN

Efficient catalytic ring-opening coupled with hydrogenation is a promising but challenging reaction for producing adipic acid (AA) from 2,5-furan dicarboxylic acid (FDCA). In this study, AA synthesis is carried out in two steps from FDCA via tetrahydrofuran-2,5-dicarboxylic acid (THFDCA) over a recyclable Ru/Al2 O3 and an ionic liquid, [MIM(CH2 )4 SO3 H]I (MIM=methylimidazolium) to deliver 99 % overall yield of AA. Ru/Al2 O3 is found to be an efficient catalyst for hydrogenation and hydrogenolysis of FDCA to deliver THFDCA and 2-hydroxyadipic acid (HAA), respectively, where ruthenium is more economically viable than well-known palladium or rhodium hydrogenation catalysts. H2 chemisorption shows that the alumina phase strongly affects the interaction between Ru nanoparticles (NPs) and supports, resulting in materials with high dispersion and small size of Ru NPs, which in turn are responsible for the high conversion of FDCA. An ionic liquid system, [MIM(CH2 )4 SO3 H]I is applied to the hydrogenolysis of THFDCA for AA production. The [MIM(CH2 )4 SO3 H]I exhibits superior activity, enables simple product isolation with high purity, and reduces the severe corrosion problems caused by the conventional hydroiodic acid catalytic system.


Asunto(s)
Líquidos Iónicos , Adipatos , Biomasa , Catálisis , Ácidos Dicarboxílicos , Furanos
7.
J Phys Chem Lett ; 12(45): 11098-11105, 2021 Nov 18.
Artículo en Inglés | MEDLINE | ID: mdl-34752106

RESUMEN

In direct H2O2 synthesis, the Pd-Au alloy was considered as a potential catalyst because of its much better performance compared to the prototype Pd; unfortunately, achieving both high activity and selectivity remains a challenge. Here, we synthesized nonconcentric Pd-Au NPs in which Au domain shells are formed only partially on Pd domain cores and tested them for direct H2O2 synthesis. It has three exposed regions of Pd, Au domains, and Pd-Au interfaces in a single NP (hence, a 3-in-1 strategy). Creating nonconcentric forms was demonstrated convincingly by density functional theory calculations. The nonconcentric Pd-Au particles exhibit high and well-balanced performances that are hard to achieve with traditional alloyed Pd-Au. The number of Pd/Au interfaces was found to be the key factor and thus was optimized by controlling the Au precursor concentrations. The hitherto underutilized structure of nonconcentric bimetallic alloys can be useful and thus should be more actively investigated for catalyst development.

8.
EMBO Rep ; 22(10): e52645, 2021 10 05.
Artículo en Inglés | MEDLINE | ID: mdl-34342389

RESUMEN

Individuals affected by infantile spasms (IS), such as those carrying mutations in an IS-linked gene, neural precursor cell expressed developmentally downregulated gene 4-like (Nedd4-2), exhibit developmental delays and learning disabilities, but the underlying mechanism is unknown. Using conditional Nedd4-2 knockout mice, we uncover that Nedd4-2 functions to maintain the excitatory synapses in hippocampal neurons and allows for late-phase long-term synaptic potentiation (L-LTP) at Schaffer collateral synapses in the hippocampus. We also find that Nedd4-2 is required for multiple forms of hippocampus-dependent learning and memory. Mechanistically, we show that loss of Nedd4-2 leads to a decrease in actin polymerization caused by reduced phosphorylation of the actin depolymerizing protein cofilin. A cell-permeable peptide promoting phosphorylation of endogenous cofilin in Nedd4-2 knockout neurons restores the number of hippocampal excitatory synapses and hippocampal L-LTP and partially restores hippocampus-dependent learning in mice. Taken together, our results reveal a novel mechanism underlying IS-associated learning disabilities and may provide information for future therapeutic strategies for IS.


Asunto(s)
Factores Despolimerizantes de la Actina , Espasmos Infantiles , Factores Despolimerizantes de la Actina/metabolismo , Animales , Modelos Animales de Enfermedad , Hipocampo/metabolismo , Humanos , Lactante , Aprendizaje , Potenciación a Largo Plazo , Ratones , Plasticidad Neuronal , Espasmos Infantiles/genética , Sinapsis/metabolismo
9.
Neurobiol Dis ; 158: 105450, 2021 10.
Artículo en Inglés | MEDLINE | ID: mdl-34303799

RESUMEN

Imbalanced neuronal excitability homeostasis is commonly observed in patients with fragile X syndrome (FXS) and the animal model of FXS, the Fmr1 KO. While alterations of neuronal intrinsic excitability and synaptic activity at the steady state in FXS have been suggested to contribute to such a deficit and ultimately the increased susceptibility to seizures in FXS, it remains largely unclear whether and how the homeostatic response of neuronal excitability following extrinsic challenges is disrupted in FXS. Our previous work has shown that the acute response following induction of endoplasmic reticulum (ER) stress can reduce neural activity and seizure susceptibility. Because many signaling pathways associated with ER stress response are mediated by Fmr1, we asked whether acute ER stress-induced reduction of neural activity and seizure susceptibility are altered in FXS. Our results first revealed that acute ER stress can trigger a protein synthesis-dependent prevention of neural network synchronization in vitro and a reduction of susceptibility to kainic acid-induced seizures in vivo in wild-type but not in Fmr1 KO mice. Mechanistically, we found that acute ER stress-induced activation of murine double minute-2 (Mdm2), ubiquitination of p53, and the subsequent transient protein synthesis are all impaired in Fmr1 KO neurons. Employing a p53 inhibitor, Pifithrin-α, to mimic p53 inactivation, we were able to blunt the increase in neural network synchronization and reduce the seizure susceptibility in Fmr1 KO mice following ER stress induction. In summary, our data revealed a novel cellular defect in Fmr1 KO mice and suggest that an impaired response to common extrinsic challenges may contribute to imbalanced neuronal excitability homeostasis in FXS.


Asunto(s)
Estrés del Retículo Endoplásmico/genética , Síndrome del Cromosoma X Frágil/genética , Convulsiones/genética , Animales , Benzotiazoles/farmacología , Proteína de la Discapacidad Intelectual del Síndrome del Cromosoma X Frágil/genética , Predisposición Genética a la Enfermedad/genética , Ácido Kaínico , Ratones , Ratones Endogámicos C57BL , Ratones Noqueados , Red Nerviosa/fisiopatología , Técnicas de Placa-Clamp , Convulsiones/inducido químicamente , Convulsiones/fisiopatología , Tolueno/análogos & derivados , Tolueno/farmacología , Proteína p53 Supresora de Tumor/antagonistas & inhibidores
10.
J Hazard Mater ; 415: 125373, 2021 Aug 05.
Artículo en Inglés | MEDLINE | ID: mdl-33765567

RESUMEN

To achieve high fuel efficiency and low emission in automobiles, it is necessary to develop highly active diesel oxidation catalysts (DOCs). Pd/CeO2 catalysts have been widely used as active catalysts for CO and C3H6 oxidation reactions. Additionally, Ag has been reported to enhance the oxygen storage capacity (OSC) of CeO2, which contributes to the oxidation ability of Pd/CeO2. In this study, Pd/Ag-CeO2 catalysts were used for CO and C3H6 oxidation reactions. When CeO2 was doped with appropriate amounts of Ag, reducibility and CO desorption rate were increased, which confirmed the high OSCs of Ag-doped catalysts. However, Ag particles were formed and the Ce3+/Ce4+ ratio decreased when CeO2 was doped with excess amounts of Ag. In addition, reduced Pd (Pd0), which is an active species for C3H6 oxidation, was formed and maintained even under oxidative reaction conditions. Since the removal of C3H6 is important for the oxidation of CO and C3H6, the catalyst with the highest Pd0 fraction (Pd/0.1Ag-CeO2 and Pd/0.3Ag-CeO2) presented improved catalytic activity. Consequently, the optimal amount of Ag enhanced the OSC of Pd/Ag-CeO2 catalysts and formed active Pd0 species under oxidative conditions, which resulted in the excellent catalytic activity of Pd/Ag-CeO2 for the CO and C3H6 oxidation reaction.

11.
J Hazard Mater ; 414: 125523, 2021 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-33676254

RESUMEN

Owing to strengthened regulations toward vehicle emissions, the use of diesel particulate filter technology to reduce particulate matter emissions has attracted significant attention. To achieve low temperature oxidation of particulate matter, numerous studies on Ag/CeO2 catalysts for soot oxidation have been reported. Herein, Ag/La-CeO2 catalysts with different La contents are synthesized and compared to analyze the effect of La. Hydrogen temperature programmed reduction analysis confirms that the reducibility increases with an increase in the La content in La-CeO2. X-ray photoelectron spectroscopy and Raman analysis confirm an increase of oxygen vacancies with La doping. Accordingly, the soot oxidation performances estimated by temperature programmed oxidation experiments increase with La doping. However, the catalytic activity of Ag/La-CeO2 exhibits a volcano trend. When an appropriate amount of La is incorporated in Ag/CeO2, peroxide generation and reducibility improve, thereby enhancing the soot oxidation performance. Conversely, the catalytic activities gradually decrease with excess La-doping. Scanning transmission electron microscopy analysis and density functional theory calculations confirm that excess amounts of La induce the sintering of Ag particles, which lead to the degradation of peroxide generation and reducibility of the catalysts. Consequently, an optimal amount of La incorporation on Ag/La-CeO2 results in the best soot oxidation performance.

12.
Environ Pollut ; 272: 116180, 2021 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-33445152

RESUMEN

Although liquid products derived from the pyrolysis of biomass are promising for the production of petroleum-like hydrocarbon fuels, the catalytic burden of hydrodeoxygenation must be reduced to achieve feasible upgrading processes. Herein, mild hydrotreating of an acid-rich biomass pyrolysis oil (bio-oil) with an unusually high total acid number (588 mg KOH/g bio-oil) was performed to stabilize the low-quality bio-oil. Ru-added TiO2-supported transition metal catalysts stabilized the bio-oil by reducing its acidity more compared to what could be achieved by Ru-free catalysts; this process also leads to lower loss of organic compounds compared to when using a Ru/TiO2 catalyst. Based on the performance of transition metal catalysts, including Ni, Co, and Cu, supported on TiO2, tungstate-zirconia, or SiO2, supported bimetallic catalysts were prepared by adding Ru to the TiO2-supported metal catalysts. The bimetallic catalysts Ru/Ni/TiO2 and Ru/Co/TiO2 exhibited good decarboxylation activity for the removal of carboxylic acids and a higher yield of organic compounds compared to that provided by Ru, which can be deemed appropriate for feedstocks when hydrodeoxygenation needs to suppress the loss of organic reactants. Using these catalysts, the carboxylic acid concentration was reduced to 319-323 mg KOH/g bio-oil with organic yields of 62-63 wt% at reaction temperatures 150-170 °C lower than the temperature required for direct conversion of carboxylic acids to alcohols or deoxygenates. The improved catalytic hydrotreating activity of Ru-added transition metals can be attributed to the high acid site densities of these catalysts along with their improved hydrogenation activities.


Asunto(s)
Biocombustibles , Dióxido de Silicio , Catálisis , Calor , Aceites de Plantas , Polifenoles
13.
J Hazard Mater ; 403: 124085, 2021 Feb 05.
Artículo en Inglés | MEDLINE | ID: mdl-33265065

RESUMEN

The effects of noble metal (M = Ag, Au, Pd, Pt, and Rh) on CeO2 in enhancing the activity toward soot oxidation were studied through experimental methods and density functional theory (DFT) calculations. Each noble metal (3 mol.%) was supported on CeO2 (M/CeO2) and the properties of the catalysts were verified by XRD, HRTEM, N2 physisorption, CO chemisorption, XPS, and H2-TPR results. The noble metal was highly dispersed over CeO2, except for Au due to the sintering of Au, and the reducibility of the catalysts was greatly improved according to degree of the interaction between each noble metal and CeO2. The activities of M/CeO2 catalysts for soot oxidation were better than that of CeO2, and followed the order Rh/CeO2 > Ag/CeO2 > Pt/CeO2 > Au/CeO2 > Pd/CeO2 > CeO2. Moreover, our DFT calculations showed that vacancy formation energy was gradually lowered in the following order: CeO2 > Pd4/CeO2 > Pt4/CeO2 > Au4/CeO2 = Ag4/CeO2 > Rh4/CeO2, which was similar order with experimental activity. In addition, the electronic states of the p and f orbitals of CeO2 were studied to compare with the occupied Ce 4f electrons, which affect the redox property. Rh/CeO2 and Ag/CeO2 showed the improved soot oxidation activity, with an enhanced ability to generate oxygen vacancy formation and oxygen adsorption and increased electron transfer. Consequently, the experimental and DFT calculation results revealed the roles of noble metals on ceria with respect to catalytic activity.

14.
Membranes (Basel) ; 10(11)2020 Nov 12.
Artículo en Inglés | MEDLINE | ID: mdl-33198322

RESUMEN

This study investigates a compact palladium membrane module (CPMM) for hydrogen purification, assembled by diffusion bonding at a low-temperature (450 °C). This CPMM resulted in hydrogen (H2) flux of 18.3 mL cm-2 min-1 with H2/N2 selectivity of over 1100. The H2 purification test using a 60% H2/40% CO2 mixed gas confirmed that the CPMM can separate H2 with a concentration of more than 99%, with a pressure difference of 5 bar. Moreover, the volume of the diffusion bonded membrane module is decreased by 81.4% than the flame-type membrane module pre-studied in our laboratory.

15.
ACS Omega ; 5(1): 197-206, 2020 Jan 14.
Artículo en Inglés | MEDLINE | ID: mdl-31956766

RESUMEN

Esters of furan dicarboxylic acids (DAFs) were synthesized by a one-pot reaction between marine biomass-derived galactaric acid and bioalcohol under solvent-free conditions and were fully characterized. The catalyst amount could be reduced without loss of reaction yields using p-xylene as the material separation agent. Also, a possible mechanism was proposed for the first time. Then the properties of four DAFs as plasticizers on the poly(vinyl chloride) (PVC) matrix were investigated. The experimental results showed that DAFs exhibit competitive efficiencies of plasticization when compared to the most commercialized plasticizer, DOP. It was found that the combination of DAFs and PVC produced homogeneous smooth-surface films, indicating miscibility between them. ATR-FTIR depicted the upshift of carbonyl absorption bands after mixing with the PVC matrix, with a magnitude of at most 18-21 cm-1. TGA, DSC, and UTM data illustrated equivalent plasticization efficiencies. Due to their small molecular weights, the investigated DAFs are more volatile. However, due to bearing an oxygen atom in the aromatic furan ring, the degree of polarization of DAFs was boosted and helped inhibit leaching into the surrounding media. In brief, these synthetic compounds have promising feasibility as biobased plasticizers. Moreover, another interesting point is that the properties of furan-2,3-dicarboxylic acid derivatives were studied for the first time and herein reported.

16.
ACS Appl Mater Interfaces ; 12(5): 6328-6335, 2020 Feb 05.
Artículo en Inglés | MEDLINE | ID: mdl-31944102

RESUMEN

To obtain high catalytic properties, finely modulating the electronic structure and active sites of catalysts is important. Herein, we report the design and economical synthesis of Pd@Pt core-shell nanoparticles for high productivity in the direct synthesis of hydrogen peroxide. Pd@Pt core-shell nanoparticles with a partially covered Pt shell on a Pd cube were synthesized using a simple direct seed-mediated growth method. The synthesized Pd@Pt core-shell nanoparticles were composed of high index faceted Pt on the corners and edges, while the Pd-Pt alloy was located on the terrace area of the Pd cubes. Because of the high-indexed Pt and Pd-Pt alloy sites, the synthesized concave Pd@Pt7 nanoparticles exhibited both high H2 conversion and H2O2 selectivity compared with Pd cubes.

17.
RSC Adv ; 10(68): 41462-41470, 2020 Nov 11.
Artículo en Inglés | MEDLINE | ID: mdl-35516558

RESUMEN

We investigated the effects of Pd precursors and preparation methods on the physicochemical properties and performance of Pd/TiO2 catalysts in the photocatalytic degradation of methyl violet. To confirm the influence of the precursors, Pd/TiO2 catalysts were prepared via chemical reduction (CR) using four different Pd precursors. Additionally, to determine the effects of preparation methods, Pd/TiO2 catalysts were fabricated using K2PdCl4 precursor via three different methods: CR, deposition-precipitation (DP), and impregnation. The CO chemisorption results showed that the catalyst prepared via DP using the K2PdCl4 precursor, i.e., Pd/TiO2_K_DP, displayed the highest Pd dispersion of 12.42% owing to the stable formation of Pd(OH)2, which strongly interacted with the -OH groups on the TiO2 support. Although the catalyst prepared via CR using the Pd(NH3)4Cl2·H2O (PA) precursor, i.e., Pd/TiO2_PA_CR, had the lowest Pd dispersion of 0.7%, it exhibited the highest absorption of 26% after 30 min in the dark. It was found that high Pd2+/Pd0 ratio in dark conditions adversely affected the absorption of MV owing to electrostatic repulsion between the cationic dyes and metal nanoparticles. However, the Pd dispersion and the specific surface area played a key role in the photocatalytic activity under UV irradiation. Pd/TiO2_K_CR with higher Pd dispersion showed the highest photocatalytic activity and reaction rate of 0.0212 min-1.

18.
RSC Adv ; 10(34): 19952-19960, 2020 May 26.
Artículo en Inglés | MEDLINE | ID: mdl-35520397

RESUMEN

When synthesizing nanoparticles in the liquid phase, polymeric materials (mainly polyvinylpyrrolidone, PVP) are applied as capping and/or stabilizing agents. The polymer layer on the nanoparticles must likely be removed since it blocks the active sites of the catalyst and inhibits mass transfer of the reactants. However, we have found that the polymer can have a positive effect on the direct synthesis of hydrogen peroxide. By testing Pd/SiO2 catalysts with different amounts of PVP, it was revealed that an adequate amount of PVP resulted in a higher rate of hydrogen peroxide production (1001 mmolH2O2 gPd -1 h-1) than pristine Pd/SiO2 did (750 mmolH2O2 gPd -1 h-1), unlike other PVP added Pd/SiO2 catalysts containing excess PVP (less than 652 mmolH2O2 gPd -1 h-1). The effect of PVP on the catalysts was examined by transmission electron microscopy, Fourier transform infrared spectroscopy, CO chemisorption, thermogravimetric analysis, and X-ray photoelectron spectroscopy. For the catalysts containing PVP, the oxidation state of the palladium 3d shifted to high binding energy due to electron transfer from Pd to the PVP molecules. Consequently, the presence of PVP on the catalysts inhibited oxygen dissociation and decomposition of the produced hydrogen peroxide, resulting in a high selectivity and high production rate of hydrogen peroxide.

19.
J Hazard Mater ; 384: 121341, 2020 02 15.
Artículo en Inglés | MEDLINE | ID: mdl-31590086

RESUMEN

To evaluate the usability of TiO2 support for silver in soot oxidation, Ag/TiO2 and Ag/CeO2 catalysts were prepared and soot oxidation experiment was performed. The catalytic activity of silver was more enhanced on P25 and rutile than on anatase and CeO2 in tight contact, as evidenced from comparing the activities of supports and silver impregnated catalysts. The reasons for the difference in active metal enhancement were elucidated by various characterization methods (TEM, H2 TPR, and XPS), and it is verified that it resulted not from dispersion of silver but from oxidation ability. On the other hand, Ag/P25 showed poor activity in loose contact because of low contact between silver and soot. To improve the loose contact activity of the Ag/P25 catalyst, CeO2 was introduced for active oxygen delivery. The synthesized CeO2-Ag/P25 catalyst showed enhanced loose contact activity when compared with Ag/P25 and Ag/CeO2 due to synergistic effects from the active oxygen supply ability of silver on P25 and the oxygen transfer ability of loaded CeO2. Thermal stability of the catalyst was identified by recycling test to 800℃, and the maintained T20 and T50 demonstrated its durability for practical use in automobile exhaust removal.

20.
Small ; 15(36): e1902090, 2019 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-31328875

RESUMEN

Recently, nonnoble-metal catalysts such as a metal coordinated to nitrogen doped in a carbon matrix have been reported to exhibit superior oxygen reduction reaction (ORR) activity in alkaline media. In this work, Co2 P nanoparticles supported on heteroatom-doped carbon catalysts (NBSCP) are developed with an eco-friendly synthesis method using bean sprouts. NBSCP can be easily synthesized through metal precursor absorption and carbonization at a high temperature. It shows a very large specific surface area with various dopants such as nitrogen, phosphorus, and sulfur derived from small organic molecules. The catalyst can exhibit activity in various electrochemical reactions. In particular, excellent performance is noted for the ORR. Compared to the commercial Pt/C, NBSCP exhibits a lower onset potential, higher current density, and superior durability. This excellent ORR activity and durability is attributable to the synergistic effect between Co2 P nanoparticles and nitrogen-doped carbon. In addition, superior performance is noted on applying NBSCP to a practical anion exchange membrane fuel cell system. Through this work, the possibility of applying an easily obtained bio-derived material to energy conversion and storage systems is demonstrated.

SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA
...