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1.
Environ Res ; 256: 119184, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-38782344

RESUMEN

The remarkable application of tin oxide in various domains is indebted to its photoelectronic merits. However, significant efforts to discover its photocatalytic potential were restricted through arduous challenges, which were the amelioration of light-harvesting and -utilizing. In fact, the uncommon light absorption energy has drawn veil over the brilliance of astounding oxidation potential, which is much more than that of TiO2. Herein, our attention was focused on the taking advantages of self-template structure for simultaneously enjoying the two sides of photoelectronic justification as well as the S-step system for eminent charge dissociation. In this regard, the optimized Cu-modified SnO2 yolk-shell ((5)YS-CuSnO) spheres were engineered through the copper modulation into glycerate-assisted metal-organic structure. As a result, the exceptional light-harvesting was achieved through desirable defects and oxygen vacancy resulted from Cu-doping, and also efficient light-utilization was obtained by the multi-scattering/reflection effect resulted from multi-shell configuration. After the effectual incorporation (40 wt⁒) of (5)YS-CuSnO was encapsulated into the V2O5-decorated wrinkled g-C3N4 lamella (VO-WCN), the dual S-step VO-WCN@(5)YS-CuSnO introduced unprecedented levofloxacin (LFC) decontamination performance, which was kinetically 5.2 and 30.2-times greater than of the (5)YS-CuSnO and bare SnO2 yolk-shell. The conspicuous fulfillment of nanocomposite was manifested in the LFC mineralization, pharmaceutical effluent treatment within 360 min, and successive cycling reactions. The fusion of the extraordinary architecture of YS-CuSnO with S-Step system not only initiates the facile and practical photocatalytic exploitation, but shade light on some undeveloped side of tin oxide.


Asunto(s)
Antibacterianos , Cobre , Fotólisis , Compuestos de Estaño , Compuestos de Estaño/química , Cobre/química , Antibacterianos/química , Compuestos de Nitrógeno/química , Grafito
2.
Sci Technol Adv Mater ; 25(1): 2309912, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38333111

RESUMEN

The control incorporation of metals in silica hollow spheres (SHSs) may bring new functions to silica mesoporous structures for applications including catalysis, sensing, molecular delivery, adsorption filtration, and storage. However, the strategies for incorporating metals, whether through pre-loading in the hollow interior or post-encapsulation in the mesoporous shell, still face challenges in achieving quantitative doping of various metals and preventing metal aggregation or channel blockage during usage. In this study, we explored the doping of different metals into silica hollow spheres based on the dissolution-regrowth process of silica. The process may promote the formation of more structural defects and functional silanol groups, which could facilitate the fixation of metals in the silica networks. With this simple and efficient approach, we successfully achieved the integration of ten diverse metal species into silica hollow sphere (SHS). Various single-metal, dual-metal, triple-metal, and quadruple-metal doped SHSs have been prepared, with the doped metals being stable and homogeneously dispersed in the structure. Based on the structural characterizations, we analyzed the influence of metal types on the morphology features of SHSs. The synergistic effects of multi-metals on the catalysis applications were also studied and compared.


Significance of this work: The control incorporation of metals in silica hollow spheres (SHSs) may bring new functions to silica mesoporous structures for applications including catalysis, sensing, molecular delivery, adsorption filtration, and storage. The incorporation of metals within SHSs is always either at the interior core or in the porous shells. The former method mainly utilizes metal nanoparticles as the core and regulates the synthesis of outer porous silica shells. The latter is primarily driven by the capillary force or intermolecular interactions with surface ligands to facilitate the post-loading of metal species in porous silica structures. The main problems associated with metal-doped SHSs include 1) controlled loading of different metals with a homogeneous distribution; 2) fixation of metal species in the structures to prevent aggregation during usage, particularly at high temperatures; 3) pore channel blockage after metal loading, which may hinder the loading of other external molecules. In this work, we developed the dissolution-regrowth of silica strategy for integrating various metals in porous SHSs (M@SHSs) by a one-pot hydrothermal process without using any anchoring molecules. Unlike other sol-gel formations, the growth rate of silica in this process is greatly reduced. It thus may bring more possibilities to introduce external metals within the silica frameworks instead of in the porous channels. By regulating the addition of metal salts in the silica nanoparticles dispersions, we have successfully synthesized stable and highly homogeneous single-metal, dual-metal, triple-metal, and quadruplemetal doped SHSs. Based on the structural characterizations, we analyzed the influence of metal types on the morphology features of SHSs. The synergistic effects of multi-metals on the catalysis applications were also studied and compared. Our results offer a facile and effective strategy for preparing multi-metals as nano-catalysts. Through proper design of the doped metals in SHSs, the structures should find more applications in catalysis, drug delivery, and adsorption with unique and enhanced properties.

3.
Molecules ; 28(24)2023 Dec 08.
Artículo en Inglés | MEDLINE | ID: mdl-38138503

RESUMEN

Visible-light-driven N2 reduction into NH3 in pure H2O provides an energy-saving alternative to the Haber-Bosch process for ammonia synthesizing. However, the thermodynamic stability of N≡N and low water solubility of N2 remain the key bottlenecks. Here, we propose a solution by developing a WO3-x hollow sphere with oxygen vacancies. Experimental analysis reveals that the hollow sphere structure greatly promotes the enrichment of N2 molecules in the inner cavity and facilitates the chemisorption of N2 onto WO3-x-HS. The outer layer's thin shell facilitates the photogenerated charge transfer and the full exposure of O vacancies as active sites. O vacancies exposed on the surface accelerate the activation of N≡N triple bonds. As such, the optimized catalyst shows a NH3 generation rate of 140.08 µmol g-1 h-1, which is 7.94 times higher than the counterpart WO3-bulk.

4.
Sensors (Basel) ; 22(17)2022 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-36081028

RESUMEN

In this study, pure zinc stannate (ZnSnO3) and bismuth (Bi)-doped ZnSnO3 composites (Bi-ZnSnO3) were synthesized via the in situ precipitation method, and their microstructures, morphologies, chemical components, sizes, and specific surface areas were characterized, followed by testing their gas sensing properties. The results revealed that Bi-ZnSnO3 showed superior gas sensing properties to n-butanol gas, with an optimal operating temperature of 300 °C, which was 50 °C lower than that of pure ZnSnO3. At this temperature, moreover, the sensitivity of Bi-ZnSnO3 to n-butanol gas at the concentration of 100 ppm reached as high as 1450.65, which was 35.57 times that (41.01) of ammonia gas, 2.93 times that (495.09) of acetone gas, 6.02 times that (241.05) of methanol gas, 2.54 times that (571.48) of formaldehyde gas, and 2.98 times that (486.58) of ethanol gas. Bi-ZnSnO3 had a highly repeatable performance. The total proportion of oxygen vacancies and chemi-adsorbed oxygen in Bi-ZnSnO3 (4 wt%) was 27.72% to 32.68% higher than that of pure ZnSnO3. Therefore, Bi-ZnSnO3 has considerable potential in detecting n-butanol gas by virtue of its excellent gas-sensing properties.


Asunto(s)
Nanosferas , 1-Butanol , Bismuto , Nanosferas/química , Oxígeno , Porosidad , Compuestos de Estaño/química
5.
Int J Mol Sci ; 23(21)2022 Oct 29.
Artículo en Inglés | MEDLINE | ID: mdl-36361949

RESUMEN

Tb-doped TiO2 (anatase) micro-hollow spheres (HSs) with nano-shells, in the range 0.00-3.00 at.% Tb, were successfully synthesized by a simultaneous chemical implantation route of both Ti and Tb cations from chlorides to a poly-styrene (PST)-co-poly-divinyl benzene (PDVB) sacrificial template, followed by controlled hydrolysis and polycondensation reactions. After water addition to the mixture of the precursors with the template, a decrease in the intensity and a shift to lower wavenumbers of the C=O absorption band in the IR spectra can indicate not only the anchoring of Ti and Tb ions to the carbonyl group of the template but also the hydrolysis of the implanted precursors. This latter process can involve a proton attack on the Ti-Cl, Tb-Cl and C=O bonds, the occupation of a vacant site by a water molecule, and then the dissociation of the dangling Ti-Cl, Tb-Cl ligands and C=O bonds. It gives rise to Ti1-xTbx[(OH)4-uClv]@PST-PDVB and Ti1-xTbx[(OH)4-y]@PST-PDVB complexes (x = 0.00, 0.0012, 0.0170 and 0.030). Finally, polycondensation of these species leads to Ti1-xTbxO2-w'@PST-PDVB compounds. After subsequent thermal removal at 550 °C of the template, the IR bands of the core (template) totally vanished and new bands were observed in the 400-900 cm-1 region which can be attributed to the metalloxane bondings (M-O, M'-O, M-O-M, M-O-M' and/or M'-O-M', being M and M' = Ti and Tb, respectively, i.e., mainly vibration modes of anatase). Then, micron-sized HSs of TiO2 and Tb-doped-TiO2 (anatase) were obtained with nano-shells according to field emission gun scanning electron microscopy (FEG-SEM) and transmission electron microscopy (TEM) observations. Furthermore, X-ray photoelectron spectroscopy (XPS) measurements confirmed the presence of Tb4+ (38.5 and 41.2% for 1.70 and 3.00 at.% Tb, respectively) in addition to Tb3+ in the resulting HSs, with increasing Tb4+ content with both Tb doping and higher calcination temperatures. Then, these HSs can be considered as rare earth (RE) co-doped systems, at least for 1.70 and 3.00 at.% Tb contents being the transition to rutile phase favored by Tb doping for those compositions. Finally, diffusion of Tb from the inner parts to the surface of the HSs with the calcination treatments was also observed by XPS.


Asunto(s)
Titanio , Agua , Titanio/química , Catálisis , Cationes
6.
Angew Chem Int Ed Engl ; 61(44): e202212045, 2022 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-36086940

RESUMEN

The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst is constructed based on CdS/MoO2 /MoS2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS2 and MoO2 are simultaneously obtained from the conversion of CdMoO4 in one step. In a photocatalytic process, the MoS2 and MoO2 function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two-step single-electron route for PA production is proposed, initiated by the cleavage of the α-C(sp3 )-H bond in the LA. The conversion of LA and the selectivity of PA can reach ca. 29 % and 95 % after a five-hour reaction, respectively.

7.
Int J Mol Sci ; 20(19)2019 Oct 04.
Artículo en Inglés | MEDLINE | ID: mdl-31590233

RESUMEN

A hollow-type spherical bacterial cellulose (HSBC) gel prepared using conventional methods cannot load particles larger than the pore size of the cellulose nanofiber network of bacterial cellulose (BC) gelatinous membranes. In this study, we prepared a HSBC gel encapsulating target substances larger than the pore size of the BC gelatinous membranes using two encapsulating methods. The first method involved producing the BC gelatinous membrane on the surface of the core that was a spherical alginate gel with a diameter of 2 to 3 mm containing the target substances. With this method, the BC gelatinous membrane was biosynthesized using Gluconacetobacter xylinus at the interface between the cell suspension attached onto the alginate gel and the silicone oil. The second method involved producing the BC gel membrane on the interface between the silicone oil and cell suspension, as well as the spherical alginate gel with a diameter of about 1 mm containing target substances. After the BC gelatinous membrane was biosynthesized, an alginate gel was dissolved in a phosphate buffer to prepare an HSBC gel with the target substances. These encapsulated substances could neither pass through the BC gelatinous membrane of the HSBC gel nor leak from the interior space of the HSBC gel. These results suggest that the HSBC gel had a molecular sieving function. The HSBC gel walls prepared using these methods were observed to be uniform and would be useful for encapsulating bioactive molecules, such as immobilized enzymes in HSBC gel, which is expected to be used as a drug carrier.


Asunto(s)
Cápsulas/química , Celulosa/análogos & derivados , Gluconacetobacter xylinus/química , Microgeles/química , Alginatos/química , Membranas Artificiales , Siliconas/química
8.
Angew Chem Int Ed Engl ; 57(48): 15707-15711, 2018 Nov 26.
Artículo en Inglés | MEDLINE | ID: mdl-30335209

RESUMEN

While bottom-up syntheses of ordered nanostructured materials at colloidal length scales have been successful at producing close-packed materials, it is more challenging to synthesize non-close-packed (ncp) structures. Here, a metal oxide nanostructure with ncp hollow sphere arrays was synthesized by combining a polymeric colloidal crystal template (CCT) with a Pechini precursor. The CCT provided defined confinement through its tetrahedral (Td ) and octahedral (Oh ) voids where the three-dimensionally (3D) ordered, ncp hollow sphere arrays formed as a result of a crystallization-induced rearrangement. This nanostructure, consisting of alternating, interconnected large and small hollow spheres, is distinct from the inverse opal structures typically generated from these CCTs. The morphology of the ncp hollow sphere arrays was retained in pseudomorphic transformations involving sulfidation and reoxidation cycling despite the segregation of zinc during these steps.

9.
Sensors (Basel) ; 17(1)2017 Jan 23.
Artículo en Inglés | MEDLINE | ID: mdl-28124997

RESUMEN

In this work, the hierarchical NiCo2O4 hollow sphere synthesized via a "coordinating etching and precipitating" process was demonstrated to exhibit intrinsic peroxidase-like activity. The peroxidase-like activity of NiCo2O4, NiO, and Co3O4 hollow spheres were comparatively studied by the catalytic oxidation reaction of 3,3,5,5-tetramethylbenzidine (TMB) in presence of H2O2, and a superior peroxidase-like activity of NiCo2O4 was confirmed by stronger absorbance at 652 nm. Furthermore, the proposed sensing platform showed commendable response to H2O2 with a linear range from 10 µM to 400 µM, and a detection limit of 0.21 µM. Cooperated with GOx, the developed novel colorimetric and visual glucose-sensing platform exhibited high selectivity, favorable reproducibility, satisfactory applicability, wide linear range (from 0.1 mM to 4.5 mM), and a low detection limit of 5.31 µM. In addition, the concentration-dependent color change would offer a better and handier way for detection of H2O2 and glucose by naked eye.


Asunto(s)
Colorimetría , Cobalto , Glucosa , Peróxido de Hidrógeno , Níquel , Oxígeno , Peroxidasa , Peroxidasas , Reproducibilidad de los Resultados
10.
ChemSusChem ; : e202400142, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38888714

RESUMEN

To enhance the inherent poor conductivity and low cycling stability of dimetallic layered double hydroxides (LDHs) materials, designing a synergistic effect between EDLC capacitors and pseudocapacitors is an efficient strategy. In this paper, we utilized a solvothermal technique employing Co-glycerate as a precursor to prepare sea urchin-like NiCo-LDH hollow spheres anchored on a 3D graphene aerogel. The unique morphology of these hollow microspheres significantly expand the specific surface area and exposes more active sites, while reducing the volume changes of materials during long-term charging and discharging processes. The 3D graphene aerogel serves as a conductive skeleton, improving the material's electrical conductivity and buffering high current. The sea urchin-like NiCo-LDH hollow spheres anchored on 3D graphene aerogel (H-NiCo-LDH@GA) has a specific surface area of 51 m2 g-1 and the ID/IG value is 1.02. The H-NiCo-LDH@GA demonstrate a significant specific capacitance of 236.8 mAh g-1 at 1 A g-1, with a remarkable capacity retention rate of 63.1 % even at 20 A g-1. Even after 8000 cycles at 10 A g-1, the capacity retention still remains at 96.3 %, presenting excellent cycling stability.

11.
Materials (Basel) ; 17(4)2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38399155

RESUMEN

The fluorinated titanium dioxide (F-TiO2) hollow spheres with varying F to Ti molar ratios were prepared by a simple one-step hydrothermal method followed by thermal processing. The diameter of the F-TiO2-0.3 hollow spheres with a nominal ratio of F:Ti = 0.3:1 was about 200-400 nm. Compared with the sensor based on pristine TiO2 sensing materials, the F-TiO2-0.3 sensor displayed an enhanced sensing performance toward gaseous formaldehyde (HCHO) vapor at room temperature under ultraviolet (UV) light irradiation. The F-TiO2-0.3 sensor demonstrated an approximately 18-fold enhanced response (1.56) compared to the pristine TiO2 sensor (0.085). The response and recovery times of the F-TiO2-0.3 sensor to 10 ppm HCHO were about 56 s and 64 s, respectively, and a limit-of-detection value of 0.5 ppm HCHO was estimated. The F-TiO2-0.3 sensor also demonstrated good repeatability and selectivity to HCHO gas under UV light irradiation. The outstanding HCHO gas-sensing properties of the F-TiO2-0.3 sensor were related to the following factors: the excitation effect caused by the UV light facilitated surface chemical reactions with analyte gas species; the hollow sphere structure provided sufficient active sites; and the surface fluoride (≡Ti-F) created additional chemisorption sites on the surface of the TiO2 material.

12.
J Colloid Interface Sci ; 657: 684-694, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38071817

RESUMEN

Given the rapidly increasing energy demand and environmental pollution, to achieve energy conservation and emission reduction, hydrogen production has emerged as a promising alternative to traditional fossil fuels because of its high gravimetric energy density, and renewable and environmentally friendly characteristics. Herein, a core-shell hollow-sphere Fe3O4@FeP@nitrogen-doped-carbon (labeled as H-Fe3O4@FeP@NC) with a dual-interface, novel morphology, and superior conductivity is prepared as an advanced bi-functional electrocatalyst for electrochemical overall water splitting using a collaborative strategy comprising of facile self-assembly and phosphating. The prepared catalyst exhibits superior electrocatalytic activity compared to H-Fe3O4@NC and H-Fe3O4 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Additionally, the overpotential of H-Fe3O4@FeP@NC for OER/HER (258/165 mV at 10 mA/cm2) is significantly lower than those of H-Fe3O4@NC (274/209 mV) and H-Fe3O4 (287/213 mV) at 10 mA/cm2. Meanwhile, the as-synthesized H-Fe3O4@FeP@NC, as an electrode pair, displays a low cell voltage of 1.69 V at 10 mA/cm2 and excellent stability after 100 h, indicating its practical application for overall water splitting. This work presents a practical and economical strategy toward the fabrication of catalyst for efficient water splitting and fuel cell.

13.
Heliyon ; 10(13): e33153, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-39040400

RESUMEN

Doping and hybridization with other semiconductors are highly effective ways to address the limitations, including their weak response to visible light and significant recombination of photogenerated carriers. In addition, the assisted carbon on the catalyst surface and the structural design have the advantage of being catalytically active. Herein, visible-light-active N-doped C/Na2Ti6O13/TiO2 hollow spheres (denoted as N-C/NTO/TiO2 HS) were successfully prepared using a facile two-step method and evaluated for methylene blue (MB) aqueous solution degradation under visible-light irradiation. The as-obtained N-C/NTO/TiO2 HS demonstrated improved photocatalytic efficiency (94 %) and pseudo-first-order kinetic degradation rate (0.023 min-1). Moreover, after three cycles of testing, N-C/NTO/TiO2 HS showed a 91 % degradation rate in its photostability. The enhanced photocatalytic performance was attributed to the combined effects of N-doping, carbon species on the surface, and the coupling of TiO2 and Na2Ti6O13 using morphology engineering. Finally, based on the experimental results, a possible photocatalytic mechanism was proposed. This study provides a rational approach toward the development of high-performance titanate-based photocatalysts for solar energy-assisted wastewater treatment.

14.
J Colloid Interface Sci ; 673: 746-755, 2024 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-38905996

RESUMEN

To clarify the key role of oxygen vacancy defects on enhancing the oxidative activity of the catalysts, metal-organic frameworks (MOFs) derived MnOX catalysts with different morphologies and oxygen vacancy defects were successfully prepared using a facile in-situ self-assembly strategy with different alkali moderators. The obtained morphologies included three-dimensional (3D) triangular cone stacked MnOX hollow sphere (MnOX-H) and 3D nanoparticle stacked MnOX nanosphere (MnOX-N). Compared to MnOX-N, MnOX-H exhibited higher activity for the oxidation of toluene (T90 = 226 °C). This was mainly due to the large number of oxygen vacancy defects and Mn4+ species in the MnOX-H catalyst. In addition, the hollow structure of MnOX-H not only facilitated toluene adsorption and activation of toluene and also provided more active sites for toluene oxidation. Reaction mechanism studies showed that the conversion of toluene to benzoate could be realized over MnOX-H catalyst during toluene adsorption at room temperature. In addition, abundant oxygen vacancy defects can accelerate the activated oxidation of toluene and the formation of oxidation products during toluene oxidation.

15.
J Colloid Interface Sci ; 633: 11-23, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36427425

RESUMEN

Visible-light-driven organic transformations boosting by localized surface plasmon resonance (LSPR) have been attracting considerable interests. Gold-palladium (Au-Pd) bimetallic nanoparticles (NPs) are considered as ideal plasmonic catalysts realizing efficient light-driven catalysis. Nevertheless, stability and adjustability of plasmonic Au-Pd NPs remain to be a challenging task. Herein, we designed the controlled Au-Pd cores in ceria (CeO2) hollow spheres (Au-Pd@h-CeO2) as nanoreactor for Suzuki cross-coupling reactions. Under visible light irradiation, the Au-Pd@h-CeO2 exhibited remarkable photocatalytic performance with a turnover frequency (TOF) value as high as 797 h-1. More impressively, the coupling reactions of aryl chlorides bearing electron-withdrawing groups proceeded better and afforded the corresponding desired products in good yields. Detailed structural, optical and photoelectrochemical characterizations unraveled that the enhanced photocatalytic efficiency of Au-Pd@h-CeO2 was attributed to the LSPR effect of controllable Au-Pd cores and their synergetic effect of hollow CeO2 shells. The merits of this hollow sphere architecture lied on as followed: (I) Incident light could be reflected and refracted between the inner cores and outer shells, which extended the trapping of incident light, and then enhanced the light harvesting efficiency; (II) the mesoporous architecture of CeO2 hollow spheres provided a huge specific surface area and numerous mesoporous channels, which could enhance the absorption of reactants and provided more active sites; (III) LSPR excitation of Au-Pd NPs and band-gap excitation of CeO2 simultaneously occurred under visible light illumination, inducing a more efficient separation and transfer of charge carriers. Furthermore, due to the confinment effect of CeO2 shells, the Au-Pd@h-CeO2 exhibited an excellent reusability after six cycles without significant deactivation of yield. Our findings provided a facile way to design highly efficient plasmonic-enhanced photocatalysts utilized for catalytic organic reactions.

16.
ACS Nano ; 17(14): 14176-14188, 2023 Jul 25.
Artículo en Inglés | MEDLINE | ID: mdl-37427983

RESUMEN

In the anodic ethanol oxidation reaction (EOR) for direct ethanol fuel cells, the coverage of hydroxide (OHads) is a major adsorbent competing with C-C bond cleavage, which is necessary for complete ethanol oxidation (C1-pathway) and durability. Beyond utilizing a less-alkaline electrolyte that causes ohmic losses, an alternative strategy to optimize OHads coverage is to intentionally exploit local pH changes near the electrocatalyst surface that are governed by a combination of released H+ during EOR and OH- mass transport from the bulk solution. Here, we manipulate the local pH swing by fine-tuning the electrode porosity with Pt1-xRhx hollow sphere electrocatalysts based on particle size (250 and 350 nm) and mass loading. With the smaller size of 250 nm, Pt0.5Rh0.5 (∼50 µg cm-2) shows a high activity of 1629 A gPtRh-1 (2488 A gPt-1) in a 0.5 M KOH-containing electrolyte, which is ∼50% higher than the most active binary catalysts to date. Moreover, a higher C1-pathway Faradaic efficiency (FE) of 38.3% and 80% longer durability are achieved with a 2-fold increase in mass loading. In the more porous electrodes, a local acidic environment created by hindered OH- mass transport better optimizes OHads coverage, providing more active sites for the desired C1-pathway and a continuous EOR.

17.
ACS Appl Mater Interfaces ; 15(28): 34044-34054, 2023 Jul 19.
Artículo en Inglés | MEDLINE | ID: mdl-37401777

RESUMEN

Solar-driven interfacial evaporation (SDIE) with excellent photothermal conversion efficiency is emerging as one of the frontier technologies for freshwater production. In this work, novel carbonized conjugate microporous polymers (CCMPs) hollow microspheres-based composite hydrogel membranes (CCMPsHM-CHM) for efficient SDIE are reported. The precursor, CMPs hollow microspheres (CMPsHM), is synthesized by an in situ Sonogashira-Hagihara cross-coupling reaction using a hard template method. The as-synthesized CCMPsHM-CHM exhibit significantly excellent properties, i.e., 3D hierarchical architecture (from micropore to macropore), superior solar light absorption (more than 89%), better thermal insulation (thermal conductivity as low as 0.32-0.42 W m-1K-1 in the wet state), superhydrophilic wettability with a water contact angle (WCA) of 0°, superior solar efficiency (up to 89-91%), a high evaporation rate of 1.48-1.51 kg m-2 h-1 under 1 sun irradiation, and excellent stability which maintains an evaporation rate of more than 80% after 10 cycles and over 83% evaporation efficiency in highly concentrated brine. In this case, the removal rate of metal ions in seawater is more than 99%, which is much lower than the ion concentration standard for drinking water set by the World Health Organization (WHO) and the United States Environmental Protection Agency (USEPA). Taking advantage of its simple and scalable manufacture, our CCMPsHM-CHM may have great potential as advanced membranes for various applications for efficient SDIE in different environments.

18.
ACS Nano ; 17(3): 3019-3036, 2023 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-36700565

RESUMEN

While development of a sodium-ion battery (SIB) cathode has been approached by various routes, research on compatible anodes for advanced SIB systems has not been sufficiently addressed. The anode materials based on titanium oxide typically show low electrical performances in SIB systems primarily due to their low electrical/ionic conductivity. Thus, in this work, layered titanium oxides were hybridized with covalent organic nanosheets (CONs), which exhibited excellent electrical conductivity, to be used as anodes in SIBs. Moreover, to enlarge the accessible areas for sodium ions, the morphology of the hybrid was formulated in the form of a hollow sphere (HS), leading to the highly enhanced ionic conductivity. This synthesis method was based on the expectation of synergetic effects since titanium oxide provides direct electrostatic sodiation sites that shield organic components and CON supports high electrical and ionic conductivity with polarizable sodiation sites. Therefore, the hybrid shows enhanced and stable electrochemical performances as an anode for up to 2600 charge/discharge cycles compared to the HS without CONs. Furthermore, the best reversible capacities obtained from the hybrid were 426.2 and 108.5 mAh/g at current densities of 100 and 6000 mA/g, which are noteworthy results for the TiO2-based material.

19.
Materials (Basel) ; 16(6)2023 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-36984184

RESUMEN

In this study, aluminum (Al) chip matrix-based synthetic foams were fabricated by hot pressing at a semi-solid (SS) temperature. The densities of the foams ranged from 2.3 to 2.63 g/cm3, confirming that the density decreased with increasing glass hollow sphere (GHS) content. These values were approximately 16% lower than the densities of Al chip alloys without GHS. The Al chip syntactic foam microstructure fabricated by the semi-solid process comprised GHS uniformly distributed around the Al chip matrix and a spherical microstructure surrounded by the Mg2Si phase in the interior. The resulting spherical microstructure contributed significantly to the improvement of mechanical properties. Mechanical characterization confirmed that the Al chip syntactic foam exhibited a compressive strength of approximately 225-288 MPa and an energy absorption capacity of 46-47 MJ/M3. These results indicate higher compressive properties than typical Al syntactic foam. The Al chip microstructure, consisting of the Mg2Si phase and GHS, acted as a load-bearing element during compression, significantly contributing to the compressive properties of the foam. An analysis was performed using an energy-dispersive spectrometer to validate the interfacial reaction between the GHS and the matrix. The results showed that MgAl2O4 was uniformly coated around GHS, which contributed not only to the strength of the matrix, but also to the mechanical properties via the appropriate interfacial reactive coating.

20.
ACS Appl Mater Interfaces ; 15(40): 47447-47462, 2023 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-37768891

RESUMEN

The self-cleaning coating has both superhydrophobic physical and photocatalytic chemical self-cleaning properties, which has attracted the wide attention of researchers in recent years. First, the flower-like hollow SiO2@TiO2 spheres with oxygen vacancies (rFHSTs) were prepared by the liquid-phase reduction method, in which several different functional components were integrated. Meanwhile, the influence mechanisms of the physical structure and chemical composition on the photocatalytic properties are discussed in detail. The results proved that rFHSTs exhibited the enhanced photoresponse range and photocatalytic degradation performance in visible light because of the synergistic effect of the microstructure (internal cavity, 3D flower-like nanosheet), SiO2/TiO2 heterojunction structure, and oxygen vacancies. After that, superhydrophobic modified rFHSTs were used as fillers to fabricate PVA/PFDTS-rFHSTs composite coatings with both physical and chemical self-cleaning properties. The self-cleaning performances and principles of the composite coating were examined and explored. The results showed that the low surface energy of the hydrophobic chain segment, the inherent particle effect, and the photocatalytic activity of rFHSTs were responsible for the superhydrophobic and photocatalytic effects, finally endowing the composite coating with self-cleaning performance. In short, this study is profound for the development and application of self-cleaning coatings with both physical and chemical performances.

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