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1.
Artículo en Inglés | MEDLINE | ID: mdl-39094052

RESUMEN

Smart materials demonstrate fascinating responses to environmental physical/chemical stimuli, including thermal, photonic, electronic, humidity, or magnetic stimuli, which have attracted intensive interest in material chemistry. However, their limited/harsh stimuli-responsive behavior or sophisticated postprocessing leads to enormous challenges for practical applications. Herein, we rationally designed and synthesized thermochromic Ni(II) organometallic [(C2H5)2NH2]2NiCl4-xBrx via a facile mechanochemical strategy, which demonstrated a reversible switch from yellow to blue color with a tunable phase-transition temperature from 75.6 to 61.7 °C. The simple electrospinning technology was applied to fabricate thermochromic Ni(II) organometallic-based nanofiber membranes for temperature monitoring. Furthermore, the organic charge-transfer cocrystal with a wide spectral absorption of 300-1950 nm and a high-efficiency photothermal conversion was combined with thermochromic Ni(II) organometallics for the desired dual-stimuli photo/thermochromism. This work supplies a new strategy for realizing multiple stimuli-responsive applications, such as thermal/light sensor displays and information storage.

2.
ACS Appl Mater Interfaces ; 16(29): 38564-38575, 2024 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-39007644

RESUMEN

In this work, graphene oxide (GO)/polymer hybrid microcapsule-loaded self-healing agents were prepared via the combination of the emulsion template method and photopolymerization technology. The incorporation of GO in the microcapsule shell not only improved the impermeability, mechanical property, and solvent resistance property of the microcapsules significantly but also endowed the microcapsules with photothermal conversion property. By incorporating GO/polymer hybrid microcapsules in water-borne epoxy resin, a novel kind of anticorrosion coating with a double self-healing property was successfully fabricated. When the coating was scratched, the linseed oil (LO) encapsulated in the microcapsules could fill the crack, and the photothermal conversion property of GO could promote the molecular chain movement of the damaged area under near-infrared (NIR) irradiation to realize the close of the crack. Based on the filling of LO and photothermal conversion-induced scratch narrowing, the "filling" and "close" double self-healing effect can be realized under temporal NIR irradiation, which could lead to the complete recovery of the scratched coating. The |Z|f=0.1Hz value of the damaged coating with GO/polymer microcapsules after double healing was comparable to that of the intact coating, which was about 4 orders of magnitude higher than that of the scratched blank coating and single self-healing coating. As to the neutral salt spray test, the scratched blank coating failed in protection after 100 h, while the healed composite coating did not show any corrosion after 300 h.

3.
ACS Nano ; 2024 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-39016025

RESUMEN

The exploitation of hierarchical carbon nanocages with superior light-to-heat conversion efficiency, together with their distinct structural, morphological, and electronic properties, in photothermal applications could provide effective solutions to long-standing challenges in diverse areas. Here, we demonstrate the discovery of pristine and nitrogen-doped hierarchical carbon nanocages as superior supports for highly loaded, small-sized Ru particles toward enhanced photothermal CO2 catalysis. A record CO production rate of 3.1 mol·gRu-1·h-1 with above 90% selectivity in flow reactors was reached for hierarchical nitrogen-doped carbon-nanocage-supported Ru clusters under 2.4 W·cm-2 illumination without external heating. Detailed studies reveal that the enhanced performance originates from the strong broadband sunlight absorption and efficient light-to-heat conversion of nanocage supports as well as the excellent intrinsic catalytic reactivity of sub-2 nm Ru particles. Our study reveals the great potential of hierarchical carbon nanocages in photothermal catalysis to reduce the fossil fuel consumption of various industrial chemical processes and stimulates interest in their exploitation for other demanding photothermal applications.

4.
Small ; : e2402510, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38984762

RESUMEN

With the rapid advancement of electronic technology, traditional textiles are challenged to keep up with the demands of wearable electronics. It is anticipated that multifunctional textile-based electronics incorporating energy storage, electromagnetic interference (EMI) shielding, and photothermal conversion are expected to alleviate this problem. Herein, a multifunctional cotton fabric with hierarchical array structure (PPy/NiCoAl-LDH/Cotton) is fabricated by the introduction of NiCoAl-layered double hydroxide (NiCoAl-LDH) nanosheet arrays on cotton fibers, followed by polymerization and growth of continuous dense polypyrrole (PPy) conductive layers. The multifunctional cotton fabric shows a high specific areal capacitance of 754.72 mF cm-2 at 5 mA cm-2 and maintains a long cycling life (80.95% retention after 1000 cycles). The symmetrical supercapacitor assembled with this fabric achieves an energy density of 20.83 Wh cm-2 and a power density of 0.23 mWcm-2. Moreover, the excellent electromagnetic interference shielding (38.83 dB), photothermal conversion (70.2 °C at 1000 mW cm-2), flexibility and durability are also possess by the multifunctional cotton fabric. Such a multifunctional cotton fabric has great potential for using in new energy, smart electronics, and thermal management applications.

5.
Nano Lett ; 2024 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-39083237

RESUMEN

Various applications related to glucose catalysis have led to the development of functional nanozymes with glucose oxidase (GOX)-like activity. However, the unsatisfactory catalytic activity of nanozymes is a major challenge for their practical applications due to their inefficient hydrogen and electron transfer. Herein, we present the synthesis of AuFe/polydopamine (PDA) superparticles that exhibit photothermal-enhanced GOX-like activity. Experimental investigations and theoretical calculations reveal that the glucose oxidation process catalyzed by AuFe/PDA follows an artificial-cofactor-mediated hydrogen atom transfer mechanism, which facilitates the generation of carbon-centered radical intermediates. Rather than depending on charged Au surfaces for thermodynamically unstable hydride transfer, Fe(III)-coordinated PDA with abundant amino and phenolic hydroxyl groups serves as cofactor mimics, facilitating both hydrogen atom and electron transfer in the catalytic process. Finally, leveraging the photothermal-enhanced GOX-like and catalase-like activities of AuFe/PDA, we establish a highly sensitive and accurate point-of-care testing blood glucose determination with exceptional anti-jamming capabilities.

6.
Artículo en Inglés | MEDLINE | ID: mdl-39048298

RESUMEN

High-entropy-alloy nanoparticles (HEA-NPs) composed of 3d transition metallic elements have attracted intensive attention in photothermal conversion regions due to their d-d interband transitions (IBTs). However, the effect arising from the unbalanced elemental ratio still needs more focus. In this work, FeCoNiCrMn HEA-NPs with different elemental ratios among Cr and Mn have been employed to clarify the impact of different composed elements on the optical absorption and photothermal conversion performance. It can be recognized that the unbalanced elemental ratio of HEA-NPs can reduce the photothermal performance. Density functional theory calculation demonstrated that d-d IBTs can be changed by the different composed element ratios, resulting in a number of insufficient filling regions around the Fermi level (±4 eV). As a result, the HEA-NPs (FeCoNiCr0.75Mn0.25) with a balanced elemental ratio exhibit the highest surface temperature of 97.6 °C under 1 sun irradiation, and the evaporation rate and energy conversion efficiency could reach 2.13 kg·m-2·h-1 and 93%, respectively, demonstrating effective solar steam generation behavior.

7.
Natl Sci Rev ; 11(7): nwae192, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-39071102

RESUMEN

Despite the discovery of a series of fullerenes and a handful of noncarbon clusters with the typical topology of I h-C60, the smallest fullerene with a large degree of curvature, C20, and its other-element counterparts are difficult to isolate experimentally. In coinage metal nanoclusters (NCs), the first all-gold fullerene, Au32, was discovered after a long-lasting pursuit, but the isolation of similar silvery fullerene structures is still challenging. Herein, we report a flying saucer-shaped 102-nuclei silver NC (Ag102) with a silvery fullerene kernel of Ag32, which is embraced by a robust cyclic anionic passivation layer of (KPO4)10. This Ag32 kernel can be viewed as a non-centered icosahedron Ag12 encaged into a dodecahedron Ag20, forming the silvery fullerene of Ag12@Ag20. The anionic layer (KPO4)10 is located at the interlayer between the Ag32 kernel and Ag70 shell, passivating the Ag32 silvery fullerene and templating the Ag70 shell. The t BuPhS- and CF3COO- ligands on the silver shell show a regioselective arrangement with the 60 t BuPhS- ligands as expanders covering the upper and lower of the flying saucer and 10 CF3COO- as terminators neatly encircling the edges of the structure. In addition, Ag102 shows excellent photothermal conversion efficiency (η) from the visible to near-infrared region (η = 67.1% ± 0.9% at 450 nm, 60.9% ± 0.9% at 660 nm and 50.2% ± 0.5% at 808 nm), rendering it a promising material for photothermal converters and potential application in remote laser ignition. This work not only captures silver kernels with the topology of the smallest fullerene C20, but also provides a pathway for incorporating alkali metal (M) into coinage metal NCs via M-oxoanions.

8.
ACS Appl Mater Interfaces ; 16(27): 35588-35603, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38924072

RESUMEN

Superhydrophobic surfaces exhibit considerable potential in road anti-icing applications due to their unique water-repellent properties. However, the nanorough structure of superhydrophobic coatings is highly susceptible to degradation under wheel rolling in practical applications. To maintain effective hydrophobicity under prolonged exposure to wheel rolling, a multilayer superhydrophobic anti-icing coating was developed. This coating utilizes antifreeze protein (AFP)-modified emulsified asphalt as the substrate with carbon nanotubes (CNTs) and silicon carbide (SiC) as surface coatings. Experimental results indicate that the inclusion of AFP enhances the viscosity of the emulsified asphalt, thereby stabilizing the nanorough structure of the coating. Even after 100 cycles of sandpaper grinding and 500 wheel rolls, the coating maintains robust hydrophobic properties. Moreover, when the coating is worn away by long-term high-strength loads, the exposed AFP-modified emulsified asphalt layer continues to exhibit effective anti-icing capabilities, significantly prolonging the complete freezing time of water droplets on its surface. Additionally, the incorporation of CNTs and SiC enhances the photothermal conversion performance, further improving the anti-icing efficiency of the coating under light irradiation. Overall, this coating shows promise for application in road anti-icing strategies.

9.
Environ Sci Pollut Res Int ; 31(30): 42640-42671, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38902444

RESUMEN

The current work investigated emerging fields for generating and consuming hydrogen and synthetic Fischer-Tropsch (FT) fuels, especially from detrimental greenhouse gases, CO2 and CH4. Technologies for syngas generation ranging from partial oxidation, auto-thermal, dry, photothermal and wet or steam reforming of methane were adequately reviewed alongside biomass valorisation for hydrogen generation, water electrolysis and climate challenges due to methane flaring, production, storage, transportation, challenges and opportunities in CO2 and CH4 utilisation. Under the same conditions, dry reforming produces more coke than steam reforming. However, combining the two techniques produces syngas with a high H2/CO ratio, which is suitable for producing long-chain hydrocarbons. Although the steam methane reforming (SMR) process has been industrialised, it is well known to consume significant energy. However, coke production via catalytic methane decomposition, the prime hindrance to large-scale implementation of these techniques for hydrogen production, could be addressed by coupling CO with CO2 conversion to alter the H2/CO ratio of syngas, increasing the reaction temperatures in dry reforming, or increasing the steam content fed in steam reforming. Optimised hydrogen production and generation of green fuels from CO2 and CH4 can be achieved by implementing these strategies.


Asunto(s)
Dióxido de Carbono , Hidrógeno , Metano , Biocombustibles
10.
Sci Rep ; 14(1): 13793, 2024 Jun 14.
Artículo en Inglés | MEDLINE | ID: mdl-38877030

RESUMEN

Solar-driven interfacial desalination technology has shown great promise in tackling the urgent global water scarcity crisis due to its ability to localize heat and its high solar-to-thermal energy conversion efficiency. For the realization of sustainable saline water desalination, the exploration of novel photothermal materials with higher water vapor generation and photothermal conversion efficiency is indispensable. In the current study, a novel 3D interconnected monolithic Ag-doped rGO network was synthesized for efficient photothermal application. The Ultraviolet-Visible-Near Infrared (UV-Vis-NIR) and FTIR analyses demonstrated that the controlled hydrothermal reduction of GO enabled the restoration of the conjugated sp2 bonded carbon network and the subsequent electrical and thermal conductivity through a significant reduction of oxygen-containing functional groups while maintaining the hydrophilicity of the composite photothermal material. In the solar simulated interfacial desalination study conducted using 3.5 wt.% saline water, the average surface temperatures of the 3D material increased from 27.1 to 54.7 °C in an hour, achieving an average net dark-excluded evaporation rate of 1.40 kg m-2 h-1 and a photothermal conversion efficiency of ~ 97.54% under 1 sun solar irradiance. In the outdoor real-world application test carried out, the surface temperature of the 3D solar evaporator reached up to 60 °C and achieved a net water evaporation rate of 1.50 kg m-2 h-1 under actual solar irradiation. The 3D interwoven porous hierarchical evaporator displayed no salt precipitation over the 54-h period monitored, demonstrating the promising salt rejection and real-world application potential for efficient desalination of saline water.

11.
Chembiochem ; : e202400334, 2024 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-38925610

RESUMEN

Hydrogels are commonly used as wound dressings to help maintain a moist environment around the wound and isolate contaminants, thus promoting healing. For irregular wounds, the slow healing process and even infection may occur due to the inability of dressings to adhere well to the wound. Prussian blue (PB) is a metal-organic framework (MOF) material with excellent photothermal conversion and superior stability. In this paper, a kind of near-infrared (NIR) light triggered in-situ polymerized antimicrobial hydrogel was prepared. The free radical initiator was encapsulated in the hollow PB by a phase change material (PCM) to maintain stability. The raised temperature triggered by NIR induced the release and decomposition of the initiator. The matrix was formed by the cross-linking of double bonds on modified chitosan. The quaternary amine groups of modified chitosan and the photothermal properties of PB enhanced the antimicrobial properties of the hydrogel. High-quality wound healing was demonstrated in the whole skin defect model. This study provides a new reference for the preparation of in-situ polymerized hydrogel dressings for irregular wounds.

12.
J Colloid Interface Sci ; 670: 395-408, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38772256

RESUMEN

Photothermal synergistic catalysis is a novel technology that converts energy. In this study, ZnIn2S4 with S-vacancy (ZIS-Vs) is combined with Nickel, Nickle Oxide and Carbon Nanofiber aggregates (Ni-NiO@CNFs) to create a multi-interface coupled photocatalyst with double Schottky barrier, double channel and mixed photothermal conversion effect. Theoretical calculation confirms that the Gibbs free energy (ΔG*H) of the S-scheme heterojunction in the composite material is -0.07 eV, which is close to 0. This promotes the adsorption of H* and accelerates the formation of H2. Internal photothermal catalysis is achieved by visible-near infrared (Vis-NIR, RT) irradiation. The internal photothermal catalytic hydrogen production rate of the best sample (0.9Ni-NiO@CNFs/ZIS-Vs) is as high as 17.24 mmol·g-1·h-1, and its photothermal conversion efficiency (η) is as high as 61.42 %. Its hydrogen production efficiency is 20.52 times that of ZIS-Vs (0.84 mmol·g-1·h-1) under visible light (Vis, RT) conditions. When the Vis-NIR light source is combined with external heating (75 ℃), the hydrogen production efficiency is further improved, and the hydrogen production efficiency (29.16 mmol·g-1·h-1) is 26.75 times that of ZIS-Vs (1.09 mmol·g-1·h-1, Vis-NIR, RT). Further analysis shows that the increase in hydrogen production resulted from the apparent activation energy (Ea) of the catalyst decreasing from 16.7 kJ·mol-1 to 9.28 kJ·mol-1. This study provides a valuable prototype for the design of an efficient photothermal synergistic catalytic system.

13.
J Colloid Interface Sci ; 670: 460-472, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-38772262

RESUMEN

Interface engineering and vacancy engineering play an important role in the surface and electronic structure of nanomaterials. The combination of the two provides a feasible way for the development of efficient photocatalytic materials. Here, we use glutathione (GSH) as a coordination molecule to design a series of CuxS nanomaterials (CuxS-GSH) rich in sulfur vacancies using a simple ultrasonic-assisted method. Interface engineering can induce amorphous structure in the crystal while controlling the formation of porous surfaces of nanomaterials, and the formation of a large number of random orientation bonds further increases the concentration of sulfur vacancies in the crystal structure. This study shows that interface engineering and vacancy engineering can enhance the light absorption ability of CuxS-GSH nanomaterials from the visible to the near-infrared region, improve the efficiency of charge transfer between CuxS groups, and promote the separation and transfer of optoelectronic electron-hole pairs. In addition, a higher specific surface area can produce a large number of active sites, and the synergistic and efficient photothermal conversion efficiency (58.01%) can jointly promote the better photocatalytic performance of CuxS-GSH nanomaterials. Based on the excellent hot carrier generation and photothermal conversion performance of CuxS-GSH under illumination, it exhibits an excellent ability to mediate the production of reactive oxygen species (ROS) through peroxide cleavage and has excellent peroxidase activity. Therefore, CuxS-GSH has been successfully developed as a nanoenzyme platform for detecting tannic acid (TA) content in tea, and convenient and rapid detection of tannic acid is achieved through the construction of a multi-model strategy. This work not only provides a new way to enhance the enzyme-like activity of nanomaterials but also provides a new prospect for the application of interface engineering and vacancy engineering in the field of photochemistry.

14.
J Colloid Interface Sci ; 671: 553-563, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38820840

RESUMEN

Recently, the solar-driven interfacial evaporation desalination has attracted more and more attentions due to the advantages of low cost, zero energy consumption, and high water purification rate, etc. One of the bottlenecks of this emerging technique lies in a lack of simple and low-cost ways to construct three-dimensional (3D) hierarchical microstructures for photothermal membranes. To this end, a two-step strategy is carried out by combining surface functionalization with substrate engineering. Firstly, a silane coupling agent 3-aminopropyltriethoxysilane (APTES) is grafted onto an ideal photothermal material of Ti3C2Tx MXene, to improve the nanochannel sizes and hydrophilicity, which are attributed to enlarged interspaces of MXene and introduced hydrophilic group e.g., -NH2 and -OH, respectively. Secondly, a low-cost and robust nonwoven fiber (NWF) substrate, which has a 3D micron-sized mesh structure with interlaced fiber stacks, is employed as the skeleton to load enough APTES-grafted MXene by a simple soaking method. Benefited from above design, the Ti3C2Tx-APTES/NWF composite membrane with a 3D hierarchical structure shows enhanced light scattering and utilization, water transport and vapor escape. A remarkable evaporation rate of 1.457 kg m-2 h-1 and an evaporation efficiency of 91.48 % are attained for a large-area (5 × 5 cm2) evaporator, and the evaporation rate is further increased to 1.672 kg m-2 h-1 for a small-area (2 × 2 cm2) device. The rejection rates of salt ions and heavy metal ions are higher than 99 % and 99.99 %, respectively, and the removal rates of organic dye molecules are nearly to 100 %. Besides, the composite photothermal membrane exhibits great stabilities in harsh conditions such as high salinities, long cycling, large light intensities, strong acid/alkali environments, and mechanical bending. Most importantly, the photothermal membrane shows a considerable cost-effectiveness of 89.4 g h-1/$. Hence, this study might promote the commercialization of solar-driven interfacial evaporation desalination by collaboratively considering surface modification and substrate engineering for MXene.

15.
ACS Appl Mater Interfaces ; 16(21): 27668-27683, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38748922

RESUMEN

Micro/nanomotors (MNMs) are miniature devices that can generate energy through chemical reactions or physical processes, utilizing this energy for movement. By virtue of their small size, self-propulsion, precise positioning within a small range, and ability to access microenvironments, MNMs have been applied in various fields including sensing, biomedical applications, and pollutant adsorption. However, the development of food-grade MNMs and their application in food delivery systems have been scarcely reported. Currently, there are various issues with the decomposition, oxidation, or inability to maintain the activity of some nutrients or bioactive substances, such as the limited application of curcumin (Cur) in food. Compared to traditional delivery systems, MNMs can adjust the transport speed and direction as needed, effectively protecting bioactive substances during delivery and achieving efficient transportation. Therefore, this study utilizes polysaccharides as the substrate, employing a simple, rapid, and pollution-free template method to prepare polysaccharide-based microtubes (PMTs) and polysaccharide-based micro/nanomotors (PMNMs). PMNMs can achieve multifunctional propulsion by modifying ferrosoferric oxide (Fe3O4), platinum (Pt), and glucose oxidase (GOx). Fe-PMNMs and Pt-PMNMs exhibit excellent photothermal conversion performance, showing promise for applications in photothermal therapy. Moreover, PMNMs can effectively deliver curcumin, achieving the effective delivery of nutrients and exerting the anti-inflammatory performance of the system.


Asunto(s)
Curcumina , Polisacáridos , Curcumina/química , Polisacáridos/química , Animales , Ratones , Platino (Metal)/química , Glucosa Oxidasa/química , Glucosa Oxidasa/metabolismo , Óxido Ferrosoférrico/química , Humanos , Ingredientes Alimentarios/análisis
16.
Nano Lett ; 24(21): 6353-6361, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38757814

RESUMEN

Polydopamine (PDA)-derived melanin-like materials exhibit significant photothermal conversion owing to their broad-spectrum light absorption. However, their low near-infrared (NIR) absorption and inadequate hydrophilicity compromise their utilization of solar energy. Herein, we developed metal-loaded poly(norepinephrine) nanoparticles (PNE NPs) by predoping metal ions (Fe3+, Mn3+, Co2+, Ca2+, Ga3+, and Mg2+) with norepinephrine, a neuron-derived biomimetic molecule, to address the limitations of PDA. The chelation between catechol and metal ions induces a ligand-to-metal charge transfer (LMCT) through the formation of donor-acceptor pairs, modulating the light absorption behavior and reducing the band gap. Under 1 sun illumination, the Fe-loaded PNE coated wood evaporator achieved a high seawater evaporation rate and efficiency of 1.75 kg m-2 h-1 and 92.4%, respectively, owing to the superior hydrophilicity and photothermal performance of PNE. Therefore, this study offers a comprehensive exploration of the role of metal ions in enhancing the photothermal properties of synthetic melanins.


Asunto(s)
Melaninas , Norepinefrina , Melaninas/química , Norepinefrina/química , Polimerizacion/efectos de la radiación , Polímeros/química , Neurotransmisores/química , Indoles/química , Oxidación-Reducción , Metales/química , Nanopartículas/química
17.
J Colloid Interface Sci ; 669: 383-392, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38718591

RESUMEN

Phase junctions exhibit great potential in photocatalytic energy conversion, yet the narrow light response region and inefficient charge transfer limit their photocatalytic performance. Herein, an anatase/rutile phase junction modified by plasmonic TiN and oxygen vacancies (TiN/(A-R-TiO2-Ov)) is prepared through an in-situ thermal transformation from TiN for efficient photothermal-assisted photocatalytic hydrogen production for the first time. The content of TiN, oxygen vacancies, and phase components in TiN/(A-R-TiO2-Ov) hybrids can be well-adjusted by tuning the heating time. The as-prepared photocatalysts display a large specific area and wide light absorption due to the synergistic effect of plasmonic excitation, oxygen vacancies, and bandgap excitations. Meanwhile, the multi-interfaces between TiN, anatase, and rutile provide built-in electric fields for efficient separation of photoinduced carriers and hot electron injection via ohmic contact and type-Ⅱ band arrangement. As a result, the TiN/(A-R-TiO2-Ov) photocatalyst shows an excellent photocatalytic hydrogen generation rate of 15.07 mmol/g/h, which is 20.6 times higher than that of titanium dioxide P25. Moreover, temperature-dependent photocatalytic tests reveal that the excellent photothermal conversion caused by plasmonic heating and crystal lattice vibrations in TiN/(A-R-TiO2-Ov) has about 25 % enhancement in photocatalysis (18.84 mmol/g/h). This work provides new inspiration for developing high-performance photocatalysts by optimizing charge transfer and photothermal conversion.

18.
Small ; : e2402993, 2024 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-38750614

RESUMEN

2D covalent organic framework (COF) materials with extended conjugated structure and periodic columnar π-arrays exhibit promising applications in organic optoelectronics. However, there is a scarcity of reports on optoelectronic COFs, mainly due to the lack of suitable π-skeletons. Here, two multi-functional optoelectronic 2D COFs DPP-TPP-COF and DPP-TBB-COF are constructed with diketopyrrolopyrrole as electron acceptor (A), and 1,3,6,8-tetraphenylpyrene and 1,3,5-triphenylbenzene as electron donor (D) through imine bonds. Both 2D COFs showed good crystallinities and AA stacking with a rhombic framework for DPP-TPP-COF and hexagonal one for DPP-TBB-COF, respectively. The electron D-A and ordered intermolecular packing structures endow the COFs with broad UV-vis absorptions and narrow bandgaps along with suitable HOMO/LUMO energy levels, resulting in multi-functional optoelectronic properties, including photothermal conversion, supercapacitor property, and ambipolar semiconducting behavior. Among them, DPP-TPP-COF exhibits a high photothermal conversion efficiency of 47% under 660 nm laser irradiation, while DPP-TBB-COF exhibits superior specific capacitance of 384 F g-1. Moreover, P-type doping and N-type doping are achieved by iodine and tetrakis(dimethylamino)ethylene on a single host COF, resulting in ambipolar semiconducting behavior. These results provide a paradigm for the application of multi-functional optoelectronic COF materials.

19.
Nanomaterials (Basel) ; 14(10)2024 May 09.
Artículo en Inglés | MEDLINE | ID: mdl-38786794

RESUMEN

Noble metal nanomaterials with a localized surface plasmon resonance effect exhibit outstanding advantages in areas such as photothermal therapy and photocatalysis. As a unique plasmonic metal nanostructure, gold nanobipyramids have been attracting much interest due to their strong specific local electric field intensity, large optical cross sections, and high refractive index sensitivity. In this study, we propose a novel three-component hetero-nanostructure composed of rough gold nanobipyramids (R-Au NBPs), Pt, and CdS. Initially, purified gold nanobipyramids are regrown to form R-Au NBPs that have a certain degree of roughness. These R-Au NBP substrates with a rough surface provide more hotspots and strengthen the intensity of localized electric fields. Subsequently, Pt and CdS nanoparticles are selectively deposited onto the surface of R-Au NBPs. Pt nanoparticles can provide more active sites. Each component of this hetero-nanostructure directly contacts others, creating multiple electron transfer channels. This novel design allows for tunable localized plasmon resonance wavelengths ranging from the visible to near-infrared regions. These factors contribute to the final superior photothermal conversion performance of the R-Au/Pt-CdS nanohybrids. Under the irradiation of near-infrared light (1064 nm), the photothermal conversion efficiency of R-Au/Pt-CdS reached 38.88%, which is 4.49, 1.5, and 1.22 times higher than that of Au NBPs, R-Au NBPs, and R-Au NBPs/Pt, respectively.

20.
ACS Appl Mater Interfaces ; 16(20): 26153-26166, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38718343

RESUMEN

Photothermal conversion materials are critical in the development of solar-driven interfacial evaporation techniques; however, achieving a high energy conversion efficiency remains challenging owing to the high cost and instability of light-absorbing materials, in addition to the difficulties of simultaneously improving light absorption while suppressing heat loss. A black silicon (Si) powder with a porous structure was prepared by chemical etching of a low-cost commercial micron-sized Al-Si alloy, and a flexible Janus black Si photothermal conversion membrane was constructed. The partially broken spherical particles and porous structure obtained after etching enhanced the refraction of light from the Si powder, imparting the prepared membrane with an average light absorption rate of 95.95% over the solar spectrum. Evaporation from the membrane increased the intermediate water content and reduced the equivalent evaporation enthalpy. The thermal conduction loss was inhibited through a one-dimensional water transport structure, and the membrane achieved a water evaporation rate of 2.17 kg m-2 h-1 and a photothermal efficiency of 94.95% under 1 sun illumination. Benefiting from the broadband absorption and high photothermal efficiency of black Si powder, surface modification of hydrophobic polydimethylsiloxane, and directional salt-out structure design, the evaporation rate of the Janus black Si membrane-based system in a 10% NaCl solution was maintained >2.10 kg m-2 h-1 after 7 days of continuous evaporation cycles. The removal rate of metal ions from simulated seawater and from practical wastewater containing complex heavy metals reached >99.9%, indicating the promising potential of black Si membrane for application in solar-driven interfacial water purification.

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