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1.
Food Chem ; 458: 140180, 2024 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-38964111

RESUMEN

Many probiotics produce functional lipids with health-promoting properties, such as short-chain fatty acids, linoleic acid and omega-3 fatty acids. They have been shown to maintain gut health, strengthen the intestinal barrier, and have anti-inflammatory and antioxidant effects. In this article, we provide an up-to-date review of the various functional lipids produced by probiotics. These probiotics can be incorporated into foods, supplements, or pharmaceuticals to produce these functional lipids in the human colon, or they can be used in industrial biotechnology processes to generate functional lipids, which are then isolated and used as ingredients. We then highlight the different physiological functions for which they may be beneficial to human health, in addition to discussing some of the challenges of incorporating probiotics into commercial products and some potential solutions to address these challenges. Finally, we highlight the importance of testing the efficacy and safety of the new generation of probiotic-enhanced products, as well as the great potential for the marketization of related products.

2.
Int J Biol Macromol ; 276(Pt 2): 133949, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-39025172

RESUMEN

Different methods of starch modification have been proposed to broaden its application. In this study, the effects of ternary mixtures of natural crosslinking agents: chitosan-betaine-vanillin and gelatin-betaine-vanillin on the properties of pea starch were explored. These combinations of substances were selected because they have complementary crosslinking mechanisms. The effects of the ternary crosslinker mixtures on the gelatinization, mechanical properties, thermal stability, and microstructure of pea starch were compared. Both combinations of crosslinkers enhanced the gelatinization viscosity, viscoelasticity, gel hardness, and thermal stability of the pea starch, by an amount that depended on the ratio of the different components in the ternary mixtures. In all cases, the crystal structure of the starch granules disappeared after gelatinization. The modified starch had a more compact and uniform microstructure than the non-modified version, especially when it was crosslinked by vanillin, gelatin, and betaine. The improvement in the gelation properties of the starch were primarily attributed to hydrogen bonding, electrostatic attraction, and Schiff base crosslinking of the various components present. Gelatin enhanced the gel strength more than chitosan, which was probably because of greater hydrogen bonding. Our findings suggest that the properties of starch can be enhanced by adding ternary mixtures of natural crosslinkers.

3.
Adv Mater ; : e2313547, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-39011781

RESUMEN

The straightforward synthesis of noble-metal-nanoparticle-decorated ordered mesoporous transition metal oxides remains a great challenge due to the difficulty of balancing the interactions between precursors and templates. Herein, a solvent-pair-enabled multicomponent coassembly (SPEMC) strategy is developed for straightforward synthesis of noble-metal-nanoparticle-decorated nitrogen-doped ordered mesoporous tungsten oxide (abbreviated as NM/N-mWO3, NM = Pt, Rh, Pd). The amphiphilic poly(ethylene oxide)-block-polystyrene (PEO-b-PS) copolymers coassemble with ammonium metatungstate (AMT) clusters and different kinds of hydrophilic noble metal precursors without phase separation. SPEMC synthesis requires no direct interaction between PEO-b-PS and AMT, thus the assembly equilibriums between noble metal precursors and PEO-b-PS can be readily controlled. The obtained NM/N-mWO3 nanocomposites possess ordered mesopores, abundant oxygen vacancies, and metal-metal oxide interfaces. As a result, the Pt/N-mWO3 sensors exhibit superior ammonia sensing performances with high sensitivity, an ultralow limit of detection (51.2 ppb), good selectivity, and long-term stability. Spectroscopic analysis reveals that ammonia is oxidized stepwise to NO, NO2 -, and NO3 - during the sensing process. Moreover, a portable wireless module based on Pt/N-mWO3 sensor can recognize ppm-level concentration of ammonia, which lays a solid foundation for its application in various fields.

4.
Food Res Int ; 187: 114459, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38763692

RESUMEN

Staple foods serve as vital nutrient sources for the human body, and chewiness is an essential aspect of food texture. Age, specific preferences, and diminished eating functions have broadened the chewiness requirements for staple foods. Therefore, comprehending the formation mechanism of chewiness in staple foods and exploring approaches to modulate it becomes imperative. This article reviewed the formation mechanisms and quality control methods for chewiness in several of the most common staple foods (rice, noodles, potatoes and bread). It initially summarized the chewiness formation mechanisms under three distinct thermal processing methods: water medium, oil medium, and air medium processing. Subsequently, proposed some effective approaches for regulating chewiness based on mechanistic changes. Optimizing raw material composition, controlling processing conditions, and adopting innovative processing techniques can be utilized. Nonetheless, the precise adjustment of staple foods' chewiness remains a challenge due to their diversity and technical study limitations. Hence, further in-depth exploration of chewiness across different staple foods is warranted.


Asunto(s)
Pan , Calidad de los Alimentos , Oryza , Solanum tuberosum , Humanos , Pan/análisis , Masticación
5.
Small ; : e2311659, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38747005

RESUMEN

The performance consistency of the gas sensor is strongly dependent on the interface binding between the sensitive materials and the electrodes. Traditional powder coating methods can inevitably lead to differences in terms of substrate-film interface interaction and device performance, affecting the stability and lifetime. Thus, efficient growth of sensitive materials on device substrates is crucial and essential to enhance the sensing performance, especially for stability. Herein, hierarchically ordered macro/mesoporous WO3 films are in situ synthesized on the electrode via a facile soft/hard dual-template strategy. Orderly arrayed uniform polystyrene (PS) microspheres with tailored size (ca. 1.2 µm) are used as a hard template, and surfactant Pluronic F127 as a soft template can co-assemble with tungsten precursor into ordered mesostructure in the interstitials of PS colloidal crystal induced by solvent evaporation. Benefiting from its rich porosity and high stability, the macro/mesoporous WO3-based sensor shows high sensitivity (Rair/Rgas = 307), fast response/recovery speed (5/9 s), and excellent selectivity (SH2S/Smax > 7) toward 50 ppm H2S gas (a biomarker for halitosis). Significantly, the sensors exhibit an extended service life with a negligible change in sensing performance within 60 days. This lab-on-device synthesis provides a platform method for constructing stable nanodevices with good consistency and high stability, which are highly desired for developing high-performance sensors.

6.
ACS Appl Mater Interfaces ; 16(14): 17563-17573, 2024 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-38551503

RESUMEN

Hydrogen generation is one of the crucial technologies to realize sustainable energy development, and the design of advanced catalysts with efficient interfacial sites and fast mass transfer is significant for hydrogen evolution. Herein, an in situ coassembly strategy was proposed to engineer a cerium-doped ordered mesoporous titanium oxide (mpCe/TiO2), of which the abundant oxygen vacancies (Ov) and highly exposed active pore walls contribute to good stability of ultrasmall Pt nanoclusters (NCs, ∼ 1.0 nm in diameter) anchored in the uniform mesopores (ca. 20 nm). Consequently, the tailored mpCe/TiO2 with 0.5 mol % Ce-doping-supported Pt NCs (Pt-mpCe/TiO2-0.5) exhibits superior H2 evolution performance toward the water-gas shift reaction with a 0.73 molH2·s-1·molPt-1 H2 evolution rate at 200 °C, which is almost 6-fold higher than the Pt-mpTiO2 (0.13 molH2·s-1·molPt-1 H2). Density functional theory calculations confirm that the structure of Ce-doped TiO2 with Ce coordinated to six O atoms by substituting Ti atoms is thermodynamically favorable without the deformation of Ti-O bonds. The Ov generated by the six O atom-coordinated Ce doping is highly active for H2O dissociation with an energy barrier of 2.18 eV, which is obviously lower than the 2.37 eV for the control TiO2. In comparison with TiO2, the resultant Ce/TiO2 support acts as a superior electron acceptor for Pt NCs and causes electron deficiency at the Pt/support interface with a 0.17 eV downshift of the Pt d-band center, showing extremely obvious electronic metal-support interaction (EMSI). As a result, abundant and hyperactive Ti3+-Ov(-Ce3+)-Ptδ+ interfacial sites are formed to significantly promote the generation of CO2 and H2 evolution. In addition, the stronger EMSI between Pt NCs and mpCe/TiO2-0.5 than that between Pt and mpTiO2 contributes to the superior self-enhanced catalytic performance during the cyclic test, where the CO conversion at 200 °C increases from 72% for the fresh catalyst to 99% for the used one. These findings reveal the subtle relationship between the mesoporous metal oxide-metal composite catalysts with unique chemical microenvironments and their catalytic performance, which is expected to inspire the design of efficient heterogeneous catalysts.

7.
Adv Mater ; 36(13): e2310155, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38100140

RESUMEN

Organic optoelectronic synaptic devices that can reliably operate in high-temperature environments (i.e., beyond 121°C) or remain stable after high-temperature treatments have significant potential in biomedical electronics and bionic robotic engineering. However, it is challenging to acquire this type of organic devices considering the thermal instability of conventional organic materials and the degradation of photoresponse mechanisms at high temperatures. Here, high-temperature synaptic phototransistors (HTSPs) based on thermally stable semiconductor polymer blends as the photosensitive layer are developed, successfully simulating fundamental optical-modulated synaptic characteristics at a wide operating temperature range from room temperature to 220°C. Robust optoelectronic performance can be observed in HTSPs even after experiencing 750 h of the double 85 testing due to the enhanced operational reliability. Using HTSPs, Morse-code optical decoding scheme and the visual object recognition capability are also verified at elevated temperatures. Furthermore, flexible HTSPs are fabricated, demonstrating an ultralow power consumption of 12.3 aJ per synaptic event at a low operating voltage of -0.05 mV. Overall, the conundrum of achieving reliable optical-modulated neuromorphic applications while balancing low power consumption can be effectively addressed. This research opens up a simple but effective avenue for the development of high-temperature and energy-efficient wearable optoelectronic devices in neuromorphic computing applications.

8.
Nat Commun ; 14(1): 8493, 2023 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-38129402

RESUMEN

Organic-inorganic molecular assembly has led to numerous nano/mesostructured materials with fantastic properties, but it is dependent on and limited to the direct interaction between host organic structure-directing molecules and guest inorganic species. Here, we report a "solvent-pair surfactants" enabled assembly (SPEA) method to achieve a general synthesis of mesostructured materials requiring no direct host-guest interaction. Taking the synthesis of mesoporous metal oxides as an example, the dimethylformamide/water solvent pairs behave as surfactants and induce the formation of mesostructured polyoxometalates/copolymers nanocomposites, which can be converted into metal oxides. This SPEA method enables the synthesis of functional ordered mesoporous metal oxides with different pore sizes, structures, compositions and tailored pore-wall microenvironments that are difficult to access via conventional direct organic-inorganic assembly. Typically, nitrogen-doped mesoporous ε-WO3 with high specific surface area, uniform mesopores and stable framework is obtained and exhibits great application potentials such as gas sensing.

9.
Int J Biol Macromol ; 253(Pt 5): 127165, 2023 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-37778592

RESUMEN

Starch has great potential to replace petroleum-based plastics in food packaging applications. However, starch films often exhibit poor mechanical and barrier properties, and are vulnerable to moisture and bacterial contamination. This study proved that the incorporation of eggshell powder (ES) enhanced the hydrogen bonding in starch-based films significantly, which contributed to improved tensile strength, Young's modulus, and water resistance of the films. The performance of ES-incorporated films could be optimized by adjusting the size, concentration, and surface property of ES in the film matrix. Notably, adsorbing epigallocatechin gallate (EGCG) on the surface of porous ES contributed to enhanced dispersibility of the fillers in the film matrix, which increased the tortuous path of light, water vapor, and oxygen have to take through the films, resulting in increased UV screening performance, water vapor and oxygen barrier property of the films by 60 %, 7.2 %, and 27.9 %, respectively. Meanwhile, loading EGCG in ES also enable superior antibacterial activity of the final films. This study suggests that eggshell fillers offer a sustainable means of improving the functional performance of starch-based films, which may increase their application as packaging materials in the food industry.


Asunto(s)
Almidón , Vapor , Animales , Cáscara de Huevo , Resistencia a la Tracción , Embalaje de Alimentos/métodos , Oxígeno , Permeabilidad
10.
Crit Rev Food Sci Nutr ; : 1-15, 2023 Sep 19.
Artículo en Inglés | MEDLINE | ID: mdl-37724782

RESUMEN

Colloidal delivery systems are widely used in the food industry to enhance the dispersibility, stability, efficacy, or bioavailability. However, when exposed to the high temperature, delivery systems are often prone to degradation, which limits its application in thermal processing. In this paper, the effects of thermal processing on the performance of traditional protein-based or starch-based delivery systems are firstly described, including the molecular structure changes of proteins, starches or lipids, and the degradation of embedded substances. These effects are unfavorable to the application of the delivery system in thermal processing. Then, strategies of improving the heat resistance of food grade colloid delivery system and their use in frying, baking and cooking food are mainly introduced. The heat resistance of the delivery system can be improved by a variety of strategies, including the development of new heat-resistant materials, the addition of heat-resistant coatings to the surface of delivery systems, the cross-linking of proteins or starches using cross-linking agents, the design of particle structures, the use of physical means such as ultrasound, or the optimization of the ingredient formula. These strategies will help to expand the application of heat-resistant delivery systems so that they can be used in real thermal processing.

11.
Small ; 19(45): e2304631, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37438544

RESUMEN

Chemiluminescence immunoassay exhibits high sensitivity and signal-to-noise ratio, thus attracting great attention in the early diagnosis and dynamic monitoring of diseases. However, the collection of conventional flash-type chemiluminescence signal (<5 s) relies heavily on automatic sampling and reading instrument. Herein, a novel core-satellite multifunctional chemiluminescence immunosensor is designed for the efficient enrichment and highly sensitive determination of cancer biomarker carcinoembryonic antigen (CEA) with enhanced and long-lasting output signal that can be conveniently recorded by a simple microplate plate reading instrument. Anti-CEA monoclonal antibody 2 (Ab2) modified Fe3 O4 @SiO2 microspheres (Fe3 O4 @SiO2 -Ab2, 370 nm in diameter) are synthesized as the core for selectively capturing and enriching target CEA in solution, and anti-human CEA monoclonal antibody 1 (Ab1) and horseradish peroxidase (HRP) co-immobilized dendritic large-mesoporous silica nanospheres (MSNs-HRP/Ab1, 80 nm in diameter, pore size: 17 nm) are synthesized as the satellite for efficient immunological recognition and signal amplification. The as-designed core-satellite magnetic chemiluminescence immunosensors exhibit a broad linear range of 0.01-20 ng mL-1 and a low detection limit of 3.0 pg mL-1 for the convenient, highly specific, and sensitive determination of CEA in human serum. Such core-satellite chemiluminescence immunosensors are expected to act as a powerful tool for in vitro detection of various biomarkers, overcome the defect of conventional chemiluminescence relying heavily on expensive and bulky automatic instruments and popularize chemiluminescence analysis to primary medical institutions and remote areas.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Humanos , Biomarcadores de Tumor , Antígeno Carcinoembrionario , Inmunoensayo , Luminiscencia , Dióxido de Silicio , Anticuerpos Monoclonales , Límite de Detección , Oro , Técnicas Electroquímicas
12.
Small ; 19(39): e2302327, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37259638

RESUMEN

Methane (CH4 ), as the vital energy resource and industrial chemicals, is highly flammable and explosive for concentrations above the explosive limit, triggering potential risks to personal and production safety. Therefore, exploiting smart gas sensors for real-time monitoring of CH4 becomes extremely important. Herein, the Pt-Pd nanoalloy functionalized mesoporous SnO2 microspheres (Pt-Pd/SnO2 ) were synthesized, which show uniform diameter (≈500 nm), high surface area (40.9-56.5 m2 g-1 ), and large mesopore size (8.8-15.8 nm). The highly dispersed Pt-Pd nanoalloys are confined in the mesopores of SnO2 , causing the generation ofoxygen defects and increasing the carrier concentration of sensitive materials. The representative Pt1 -Pd4 /SnO2 exhibits superior CH4 sensing performance with ultrahigh response (Ra /Rg = 21.33 to 3000 ppm), fast response/recovery speed (4/9 s), as well as outstanding stability. Spectroscopic analyses imply that such an excellent CH4 sensing process involves the fast conversion of CH4 into formic acid and CO intermediates, and finally into CO2 . Density functional theory (DFT) calculations reveal that the attractive covalent bonding interaction and rapid electron transfer between the Pt-Pd nanoalloys and SnO2 support, dramatically promote the orbital hybridization of Pd4 sites and adsorbed CH4 molecules, enhancing the catalytic activation of CH4 over the sensing layer.

13.
Small ; 19(32): e2301011, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37066705

RESUMEN

Site-selective and partial decoration of supported metal nanoparticles (NPs) with transition metal oxides (e.g., FeOx ) can remarkably improve its catalytic performance and maintain the functions of the carrier. However, it is challenging to selectively deposit transition metal oxides on the metal NPs embedded in the mesopores of supporting matrix through conventional deposition method. Herein, a restricted in situ site-selective modification strategy utilizing poly(ethylene oxide)-block-polystyrene (PEO-b-PS) micellar nanoreactors is proposed to overcome such an obstacle. The PEO shell of PEO-b-PS micelles interacts with the hydrolyzed tungsten salts and silica precursors, while the hydrophobic organoplatinum complex and ferrocene are confined in the hydrophobic PS core. The thermal treatment leads to mesoporous SiO2 /WO3-x framework, and meanwhile FeOx nanolayers are in situ partially deposited on the supported Pt NPs due to the strong metal-support interaction between FeOx and Pt. The selective modification of Pt NPs with FeOx makes the Pt NPs present an electron-deficient state, which promotes the mobility of CO and activates the oxidation of CO. Therefore, mesoporous SiO2 /WO3-x -FeOx /Pt based gas sensors show a high sensitivity (31 ± 2 in 50 ppm of CO), excellent selectivity, and fast response time (3.6 s to 25 ppm) to CO gas at low operating temperature (66 °C, 74% relative humidity).

14.
ACS Appl Mater Interfaces ; 15(12): 15721-15731, 2023 Mar 29.
Artículo en Inglés | MEDLINE | ID: mdl-36917766

RESUMEN

Hydrogen as an important clean energy source with a high energy density has attracted extensive attention in fuel cell vehicles and industrial production. However, considering its flammable and explosive property, gas sensors are desperately desired to efficiently monitor H2 concentration in practical applications. Herein, a facile polymerization-induced aggregation strategy was proposed to synthesize uniform Si-doped mesoporous WO3 (Si-mWO3) microspheres with tunable sizes. The polymerization of the melamine-formaldehyde resin prepolymer (MF prepolymer) in the presence of silicotungstic acid hydrate (abbreviated as H4SiW) leads to uniform MF/H4SiW hybrid microspheres, which can be converted into Si-mWO3 microspheres through a simple thermal decomposition treatment process. In addition, benefiting from the pore confinement effect, monodispersed Pd-decorated Si-mWO3 microspheres (Pd/Si-mWO3) were subsequently synthesized and applied as sensitive materials for the sensing and detection of hydrogen. Owing to the oxygen spillover effect of Pd nanoparticles, Pd/Si-mWO3 enables adsorption of more oxygen anions than pure mWO3. These Pd nanoparticles dispersed on the surface of Si-mWO3 accelerated the dissociation of hydrogen and promoted charge transfer between Pd nanoparticles and WO3 crystal particles, which enhanced the sensing sensitivity toward H2. As a result, the gas sensor based on Pd/Si-mWO3 microspheres exhibited excellent selectivity and sensitivity (Rair/Rgas = 33.5) to 50 ppm H2 at a relatively low operating temperature (210 °C), which was 30 times higher than that of the pure Si-mWO3 sensor. To develop intelligent sensors, a portable sensor module based on Pd/Si-mWO3 in combination with wireless Bluetooth connection was designed, which achieved real-time monitoring of H2 concentration, opening up the possibility for use as intelligent H2 sensors.

15.
Adv Sci (Weinh) ; : e2204810, 2022 Nov 14.
Artículo en Inglés | MEDLINE | ID: mdl-36373719

RESUMEN

With the emerging of the Internet of Things, chemiresistive gas sensors have been extensively applied in industrial production, food safety, medical diagnosis, and environment detection, etc. Considerable efforts have been devoted to improving the gas-sensing performance through tailoring the structure, functions, defects and electrical conductivity of sensitive materials. Among the numerous sensitive materials, mesoporous semiconductor metal oxides possess unparalleled properties, including tunable pore size, high specific surface area, abundant metal-oxygen bonds, and rapid mass transfer/diffusion behavior (Knudsen diffusion), which have been regarded as the most potential sensitive materials. Herein, the synthesis strategies for mesoporous metal oxides are overviewed, the classical functionalization techniques of sensitive materials are also systemically summarized as a highlight, including construction of mesoporous structure, regulation of micro-nano structure (i.e., heterojunctions), noble metal sensitization (e.g., Au, Pt, Ag, Pd) and heteroatomic doping (e.g., C, N, Si, S). In addition, the structure-function relationship of sensitive materials has been discussed at molecular-atomic level, especially for the chemical sensitization effect, elucidating the interface adsorption/catalytic mechanism. Moreover, the challenges and perspectives are proposed, which will open a new door for the development of intelligent gas sensor in various applications.

16.
Adv Sci (Weinh) ; 9(33): e2203594, 2022 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-36116122

RESUMEN

With the development of internet of things and artificial intelligence electronics, metal oxide semiconductor (MOS)-based sensing materials have attracted increasing attention from both fundamental research and practical applications. MOS materials possess intrinsic physicochemical properties, tunable compositions, and electronic structure, and are particularly suitable for integration and miniaturization in developing chemiresistive gas sensors. During sensing processes, the dynamic gas-solid interface interactions play crucial roles in improving sensors' performance, and most studies emphasize the gas-MOS chemical reactions. Herein, from a new view angle focusing more on physical gas-solid interactions during gas sensing, basic theory overview and latest progress for the dynamic process of gas molecules including adsorption, desorption, and diffusion, are systematically summarized and elucidated. The unique electronic sensing mechanisms are also discussed from various aspects including molecular interaction models, gas diffusion mechanism, and interfacial reaction behaviors, where structure-activity relationship and diffusion behavior are overviewed in detail. Especially, the surface adsorption-desorption dynamics are discussed and evaluated, and their potential effects on sensing performance are elucidated from the gas-solid interfacial regulation perspective. Finally, the prospect for further research directions in improving gas dynamic processes in MOS gas sensors is discussed, aiming to supplement the approaches for the development of high-performance MOS gas sensors.

17.
ACS Cent Sci ; 8(12): 1633-1645, 2022 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-36589882

RESUMEN

As an important kind of emerging heterogeneous catalyst for sustainable chemical processes, supported metal cluster (SMC) catalysts have received great attention for their outstanding activity; however, the easy aggregation of metal clusters due to their migration along the substrate's surface usually deteriorates their activity and even causes catalyst failure during cycling. Herein, stable Pt nanoclusters (NCs, ∼1.06 nm) are homogeneously confined in the uniform spherical mesopores of mesoporous titania (mpTiO2) by the interaction between Pt NCs and metal oxide pore walls made of polycrystalline anatase TiO2. The obtained Pt-mpTiO2 exhibits excellent stability with well-retained CO conversion (∼95.0%) and Pt NCs (∼1.20 nm) in the long term water-gas shift (WGS) reaction. More importantly, the Pt-mpTiO2 displays an unusual increasing activity during the cyclic catalyzing WGS reaction, which was found to stem from the in situ generation of interfacial active sites (Ti3+-Ov-Ptδ+) by the reduction effect of spillover hydrogen generated at the stably supported Pt NCs. The Pt-mpTiO2 catalysts also show superior performance toward the selective hydrogenation of furfural to 2-methylfuran. This work discloses an efficient and robust Pt-mpTiO2 catalyst and systematically elucidates the mechanism underlying its unique catalytic activity, which helps to design stable SMC catalysts with self-enhancing interfacial activity in sustainable heterogeneous catalysis.

18.
ACS Cent Sci ; 7(11): 1885-1897, 2021 Nov 24.
Artículo en Inglés | MEDLINE | ID: mdl-34841059

RESUMEN

Mesoporous materials have been extensively studied for various applications due to their high specific surface areas and well-interconnected uniform nanopores. Great attention has been paid to synthesizing stable functional mesoporous metal oxides for catalysis, energy storage and conversion, chemical sensing, and so forth. Heteroatom doping and surface modification of metal oxides are typical routes to improve their performance. However, it still remains challenging to directly and conveniently synthesize mesoporous metal oxides with both a specific functionalized surface and heteroatom-doped framework. Here, we report a one-step multicomponent coassembly to synthesize Pt nanoparticle-decorated Si-doped WO3 nanowires interwoven into 3D mesoporous superstructures (Pt/Si-WO3 NWIMSs) by using amphiphilic poly(ethylene oxide)-block-polystyrene (PEO-b-PS), Keggin polyoxometalates (H4SiW12O40) and hydrophobic (1,5-cyclooctadiene)dimethylplatinum(II) as the as structure-directing agent, tungsten precursor and platinum source, respectively. The Pt/Si-WO3 NWIMSs exhibit a unique mesoporous structure consisting of 3D interwoven Si-doped WO3 nanowires with surfaces homogeneously decorated by Pt nanoparticles. Because of the highly porous structure, excellent transport of carriers in nanowires, and rich WO3/Pt active interfaces, the semiconductor gas sensors based on Pt/Si-WO3 NWIMSs show excellent sensing properties toward ethanol at low temperature (100 °C) with high sensitivity (S = 93 vs 50 ppm), low detection limit (0.5 ppm), fast response-recovery speed (17-7 s), excellent selectivity, and long-term stability.

19.
Small ; 17(39): e2103176, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-34405523

RESUMEN

2D transition metal oxides (TMO) nanosheets have attracted considerable attention in both fundamental research and practical applications. Herein, a convenient programmable and scalable carbonate crystals templating synthesis is developed to produce high-quality self-hybrid TMO nanosheets (Si-WO3- x , Tax Oy , Mnx Oy ) and their respective polymetallic oxide hybrid nanosheets with tunable composition, low-cost and high-yield. Taking tungsten oxide nanosheets as example, silicotungstic acid precursor is in situ converted into tungsten oxide nanosheets like scales on the surface of calcium carbonate crystals through the simple soaking-drying-calcination process, and after selectively dissolving calcium carbonate by etching, the dispersive tungsten oxide nanosheets with unique self-hybrid Si-doped h-WO3 /ε-WO3 /WO2 compositions are obtained, which show excellent acetone gas-sensing performances at low temperatures. This carbonate-template method opens up the possibility to economically produce various functional TMO nanosheets with specific compositions for diverse applications.

20.
ACS Appl Mater Interfaces ; 13(44): 51933-51944, 2021 Nov 10.
Artículo en Inglés | MEDLINE | ID: mdl-34110132

RESUMEN

Zinc oxide (ZnO) as a commonly used semiconductor material has aroused extensive research attention in various fields, such as field-effect transistors, solar cells, luminescent devices, and sensors, because of its excellent light-electrical features and large exciton bonding energy. Herein, ultrasmall Au nanoparticles with tunable size decorated mesoporous ZnO nanospheres were synthesized via facile formaldehyde-assisted metal-ligand cross-linking strategy, where these active Au species could be transferred into Au nanoparticles in the frameworks by various reduction strategies. Typically, mesoporous ZnO-Au with a photoreduction technique showed superior ethanol sensing performance (ca. 159 for 50 ppm at 200 °C) because of its high surface area, dual-mesoporous structure, and interface effect (electron effect, surface catalytic/adsorption). Moreover, the mesoporous ZnO-Au composites by photoreduction show much better performance than those via H2 reduction and NaBH4 reduction, which is ascribed to the providential size of Au nanoparticles (ca. 6.6 nm) and abundant oxygen defects in the composites. In particular, the selectivity and sensitivity of mesoporous ZnO-Au far exceeds those of materials loaded with other noble metals (Pt, Pd, and Ag). The sensing mechanism of mesoporous ZnO-Au for ethanol is attributed to classical surface adsorption/catalytic reaction, where strong sensitization effect (electron and chemical) and the spillover effect of Au nanoparticles in the catalytic reaction cause superior ethanol sensing performances. In situ FTIR and GC-MS measurement revealed that the catalytic oxidation of ethanol follows the process of dehydrogenation and deep oxidation, that is, dehydrogenation to acetaldehyde, and then further oxidation to carbon dioxide and water.

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