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1.
Adv Sci (Weinh) ; 11(22): e2400275, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38504472

RESUMEN

Energy loss in perovskite grain boundaries (GBs) is a primary limitation toward high-efficiency perovskite solar cells (PSCs). Two critical strategies to address this issue are high-quality crystallization and passivation of GBs. However, the established methods are generally carried out discretely due to the complicated mechanisms of grain growth and defect formation. In this study, a combined method is proposed by introducing 3,4,5-Trifluoroaniline iodide (TFAI) into the perovskite precursor. The TFAI triggers the union of nano-sized colloids into microclusters and facilitates the complete phase transition of α-FAPbI3 at room temperature. The controlled chemical reactivity and strong steric hindrance effect enable the fixed location of TFAI and suppress defects at GBs. This combination of well-crystallized perovskite grains and effectively passivated GBs leads to an improvement in the open circuit voltage (Voc) of PSCs from 1.08 V to 1.17 V, which is one of the highest recorded Voc without interface modification. The TFAI-incorporated device achieved a champion PCE of 24.81%. The device maintained a steady power output near its maximum power output point, showing almost no decay over 280 h testing without pre-processing.

2.
Nanoscale Adv ; 6(2): 559-569, 2024 Jan 16.
Artículo en Inglés | MEDLINE | ID: mdl-38235083

RESUMEN

Optoelectronic synaptic transistors are attractive for applications in next-generation brain-like computation systems, especially for their visible-light operation and in-sensor computing capabilities. However, from a material perspective, it is difficult to build a device that meets expectations in terms of both its functions and power consumption, prompting the call for greater innovation in materials and device construction. In this study, we innovatively combined a novel perovskite carrier supply layer with an Al/MoO3 interface carrier regulatory layer to fabricate optoelectronic synaptic devices, namely Al/MoO3/CsFAMA/ITO transistors. The device could mimic a variety of biological synaptic functions and required ultralow-power consumption during operation with an ultrafast speed of >0.1 µs under an optical stimulus of about 3 fJ, which is equivalent to biological synapses. Moreover, Pavlovian conditioning and visual perception tasks could be implemented using the spike-number-dependent plasticity (SNDP) and spike-rate-dependent plasticity (SRDP). This study suggests that the proposed CsFAMA synapse with an Al/MoO3 interface has the potential for ultralow-power neuromorphic information processing.

3.
J Phys Chem Lett ; 15(4): 1112-1120, 2024 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-38262437

RESUMEN

Quasi-two-dimensional (2D) perovskite light-emitting diodes are promising light sources for color display and lighting. However, poor carrier injection and transport between the bottom hole transport layer (HTL) and perovskite limit the device performance. Here we demonstrate a simple and effective way to modify the HTL for enhancing the performance of perovskite light-emitting diodes (PeLEDs). An electrolyte K2SO4 is used to mix with poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) as the hole transport layer. The K+ doping helped the quasi-2D perovskite phases grow vertically along the interface of the PEDOT:PSS, fine-modulate the phase distribution, and simultaneously reduce the defect density of quasi-2D perovskites. It also significantly reduced the exciton quenching and injection barrier at PEDOT:PSS and quasi-2D perovskite interface. The optimized green PeLEDs with the K2SO4 doped PEDOT:PSS HTL showed a maximum luminance of 17185 cd/m2 which is almost 4.7 times brighter than the control one, with a maximum external quantum efficiency of 18.64%.

4.
Adv Mater ; 35(46): e2302298, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37578639

RESUMEN

Perovskite single-crystal redissolution (PSCR) strategy is highly desired for efficient formamidinium lead triiodide (FAPbI3 ) perovskite photovoltaics with enhanced phase purity, improved film quality, low trap-state density, and good stability. However, the phase transition and crystallization dynamics of FAPbI3 remain unclear in the PSCR process compared to the conventional fabrication from the mixing of precursor materials. In this work, a green-solvent-assisted (GSA) method is employed to synthesize centimeter-sized α-FAPbI3 single crystals, which serve as the high-purity precursor to fabricate perovskite films. The α-FAPbI3 PSCR strategy facilitates direct α-phase formation and inhibits the complex intermediate phases monitored by in situ grazing-incidence wide-angle X-ray scattering. Moreover, the α-phase stability is prolonged due to the relaxation of the residual lattice strain through the isotropic orientation phase growth. Consequently, the GSA-assisted PSCR strategy effectively promotes crystallization and suppresses non-radiative recombination in perovskite solar cells, which boosts the device efficiency from 22.08% to 23.92% with significantly enhanced open circuit voltage. These findings provide deeper insight into the PSCR process in terms of its efficacy in phase formation and lattice strain release. The green low-cost solvent may also offer a new and ideal solvent candidate for large-scale production of perovskite photovoltaics.

5.
ACS Appl Mater Interfaces ; 15(30): 36447-36456, 2023 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-37485977

RESUMEN

Preferred crystalline orientation at the surface of quasi-2D organic-inorganic halide perovskites is crucial to promote vertical carrier transport and interface carrier extraction, which further contribute to device efficiency and stability in photovoltaic applications. However, loose unoriented and defective surfaces are inevitably formed in the crystallization process, especially with the introduction of bulky organic cations into the quasi-2D perovskites. Here, a facile and effective surface polishing method using a natural-friendly green solvent, 2,2,2-trifluoroethanol, is proposed to reconstruct the surface. After solvent polishing, the randomly oriented phases containing trap sites on the surface are successfully removed, and the compact vertical-oriented phases underneath are revealed with less defectiveness and better smoothness, which greatly facilitates carrier transport and interfacial charge extraction. Consequently, the green solvent polished devices show a boosting efficiency of 18.38% with a high open-circuit voltage of 1.21 V. The devices also show improved storage and operational stability.

6.
Environ Pollut ; 319: 121005, 2023 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-36608731

RESUMEN

The organic modification of three-dimensional porous diatom frustules (biosilica) and their fossils (diatomite) is promising in heavy metal adsorption. However, the preparation of such materials involves complex processes, high costs, and environmental hazards. In this study, organic-biosilica composites based on in situ self-modification of diatoms were prepared by freeze-drying pretreatment. Freeze-drying resulted in the release of the intercellular organic components of diatoms, followed by loading on the surface of their diatom frustules. The bio-adsorbent exhibits outstanding Cd2+ adsorption capacity (up to 220.3 mg/g). The adsorption isotherms fitted the Langmuir model and the maximum adsorption capacity was 4 times greater than that of diatom biosilica (54.1 mg/g). The adsorption kinetics of Cd2+ was adequately described by a pseudo-second-order model and reached equilibrium within 30 min. By combining focused ion beam thinning with transmission electron microscopy-energy dispersive X-ray spectroscopy, the internal structure of the composite and the Cd2+ distribution were investigated. The results showed that the organic matter of the composite adsorbed approximately 10 times more Cd2+ than inorganic biosilica. The adsorption mechanism was dominated by complexation between the abundant organic functional groups (amide, carboxyl, and amino groups) on the surfaces of composite and Cd2+. The bio-adsorbent was demonstrated to have wide applicability in the presence of competitive cations (Na+, K+, Ca2+, and Mg2+) and under a wide range of pH (3-10) conditions. Thus, the self-modification of diatoms offers a promising organic-inorganic composite for heavy metal remediation.


Asunto(s)
Diatomeas , Metales Pesados , Contaminantes Químicos del Agua , Diatomeas/química , Cadmio , Microscopía Electrónica de Transmisión , Cationes , Adsorción , Cinética , Concentración de Iones de Hidrógeno
7.
Adv Sci (Weinh) ; 10(5): e2205879, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36494090

RESUMEN

Realization of remote wearable health monitoring (RWHM) technology for the flexible photodiodes is highly desirable in remote-sensing healthcare systems used in space stations, oceans, and forecasting warning, which demands high external quantum efficiency (EQE) and detectivity in NIR region. Traditional inorganic photodetectors (PDs) are mechanically rigid and expensive while the widely reported solution-processed mixed tin-lead (MSP) perovskite photodetectors (PPDs) exhibit a trade-off between EQE and detectivity in the NIR region. Herein, a novel functional passivating antioxidant (FPA) strategy has been introduced for the first time to simultaneously improve crystallization, restrain Sn2+ oxidization, and reduce defects in MSP perovskite films by multiple interactions between thiophene-2-carbohydrazide (TAH) molecules and cations/anions in MSP perovskite. The resultant solution-processed rigid mixed Sn-Pb PPD simultaneously achieves high EQE (75.4% at 840 nm), detectivity (1.8 × 1012 Jones at 840 nm), ultrafast response time (trise /tfall = 94 ns/97 ns), and improved stability. This work also highlights the demonstration of the first flexible photodiode using MSP perovskite and FPA strategy with remarkably high EQE (75% at 840 nm), and operational stability. Most importantly, the RWHM is implemented for the first time in the PIN MSP perovskite photodiodes to remotely monitor the heart rate of humans at rest and after-run conditions.

8.
ACS Appl Mater Interfaces ; 14(46): 52007-52016, 2022 Nov 23.
Artículo en Inglés | MEDLINE | ID: mdl-36349638

RESUMEN

It is essential to release annealing induced strain during the crystallization process to realize efficient and stable perovskite solar cells (PSCs), which does not seem achievable using the conventional annealing process. Here we report a novel and facile thermal gradient assisted crystallization strategy by simply introducing a slant angle between the preheated hot plate and the substrate. A distinct crystallization sequence resulted along the in-plane direction pointing from the hot side to the cool side, which effectively reduced the crystallization rate, controlled the perovskite grain growth, and released the in-plane tensile strain. Moreover, this strategy enabled uniform strain distribution in the vertical direction and assisted in reducing the defects and aligning the energy bands. The corresponding device demonstrated champion power conversion efficiencies (PCEs) of 23.70% and 21.04% on the rigid and flexible substrates, respectively. These highly stable rigid devices retained 97% of the initial PCE after 1097 h of storage and more than 80% of the initial PCE after 1000 h of continuous operation at the maximum power point. This novel strategy opens a simple and effective avenue to improve the quality of perovskite films and photovoltaic devices via strain modulation and defect passivation.

9.
Phys Chem Chem Phys ; 24(13): 7969-7977, 2022 Mar 30.
Artículo en Inglés | MEDLINE | ID: mdl-35311859

RESUMEN

Quasi-two-dimensional (quasi-2D) perovskites are emerging as promising materials for highly stable light-emitting diodes (LEDs). However, their lower charge transport mobilities and higher defect densities may constrain their light-emitting efficiency. Here, we combine an excessive-salt-assisted (ESA) process with antisolvent treatments to inhibit the defects in Dion-Jacobson-type perovskite LEDs. Such a method could improve the film quality and recombination efficiency. By further investigation, we found that artificially building a bulk junction interface and enhancing surface polarization could play a more important role in promoting the ability of charge carrier injection and recombination for high-performance LED devices. Accordingly, the DJ-type quasi-2D perovskite LED can achieve a high external quantum efficiency (EQE) of 7.1%.

10.
Materials (Basel) ; 15(3)2022 Jan 27.
Artículo en Inglés | MEDLINE | ID: mdl-35160919

RESUMEN

Calcium carbide residue (CCR) is a solid waste resulting from acetylene gas production. In this study, CCR was used as an alkali activator to prepare fly ash (FA)-based geopolymers without any alkali supplementation. We studied the factors (FA/CCR ratio, curing temperature, and water/binder ratio) influencing the mechanical property of FA/CCR-based geopolymers. The compressive strength results showed that, by optimizing these three factors, the FA/CCR mixture has great potential for use as a cementitious material and geopolymer with a dense microstructure having a maximal compressive strength of 17.5 MPa. The geopolymers' chemical structure, microstructure, and chemical composition were characterized and determined by a combination of techniques. All these results revealed that amorphous C-(A)-S-H (calcium (aluminate) silicate hydrate) gels mainly formed after geopolymerization resulting from the reaction of FA and CCR. In addition, some crystallines, such as ettringite and monosulfate, were also formed. Further, geopolymers prepared with a suitable FA/CCR ratio (1:1 or 1:2) possessed a compact microstructure because of their sufficient reactive SiO2 and Al2O3 and high-enough alkalinity, responsible for higher content of C-(A)-S-H formation and better mechanical property. Too high curing temperature or water content induced the formation of a loosely bound geopolymer matrix that strongly weakens its mechanical property.

11.
J Phys Chem Lett ; 11(18): 7583-7589, 2020 Sep 17.
Artículo en Inglés | MEDLINE | ID: mdl-32808791

RESUMEN

As a new kind of highly efficient luminescent materials, quasi-two-dimensional (quasi-2D) perovskites show great potential in industrial display applications. In this work, the poling methods are used in modulating the phase arrangement in quasi-2D perovskite light-emitting diodes (PeLEDs). We find the effective modulation of different phase components in uniform arrangement can enhance both brightness and current efficiency to 30 810 cd/m2 and 8.3 cd/A, about 2 times in comparison to results for the control devices. Upon further investigation by optical and impedance spectroscopy, we find the phase modulation can improve the balance of charge carrier injection without sacrificing the transport ability. We believe our studies can provide new inspiration on the influence of phase arrangement in PeLED devices.

12.
ACS Appl Mater Interfaces ; 12(4): 5120-5127, 2020 Jan 29.
Artículo en Inglés | MEDLINE | ID: mdl-31902207

RESUMEN

These days, organic-inorganic hybrid perovskites (OIHP) and non-fullerene acceptor (NFA) molecules are all at the frontiers of research and development in the domain of photovoltaics. A careful design and use of inorganic transparent metal oxides with wide band gaps as electron and hole transport layers are critically important for highly efficient and stable solar cells. As one of the most favorable electron transport materials, tin oxide (SnO2), which has been frequently utilized in highly efficient OIHP solar cells, is rarely seen in the application of NFA organic bulk heterojunction (BHJ) solar cells. To appropriately tailor an interface of SnO2 and an organic blend, while to make them compatible and useful may offer some opportunities for achieving higher efficiencies and longer lifetimes. In fact, there is still a lack of a method to solve the problem. Herein, a unique way is developed by implementing a surface decoration nanostructure such as low dimensional MAPbI3 perovskite nanowires (PeNWs) at the interface of SnO2 and the organic blend such as PBDB-T-SF:IT-4F. Such an interface functions well for the improvement of photovoltaic performance for the organic solar cell of the structure ITO(glass)/SnO2/PeNWs/PBDB-T-SF:IT-4F/MoO3/Ag. Experimental results indicate that the electron-hole dissociation, charge extraction, and photo-absorption ability of the organic solar cell can be improved significantly. The inside generation of the photocurrent is explored by the magneto-photocurrent method. Finally, the solar cell exhibits more than 80% power conversion efficiencies even after 20 days, which suggests the merits of having both SnO2 and PeNWs in the NFA-based organic solar cell.

13.
Nat Commun ; 10(1): 4829, 2019 10 23.
Artículo en Inglés | MEDLINE | ID: mdl-31645556

RESUMEN

Diatoms play an important role in marine biogeochemical cycle of aluminum (Al), as dissolved Al is taken up by diatoms to build their siliceous frustules and is involved in the sedimentation of diatomaceous biogenic silica (BSi). The Al incorporation in BSi facilitates decreasing the dissolution of marine BSi and thus substantially influences the biochemical processes driven by diatoms, such as CO2 sequestration. However, the role of lake BSi in the terrestrial biochemical Al cycle has not been explored, though lakes represent the second-largest sink for BSi. By identifying the previously unexplored high Al/Si atomic ratios (up to 0.052) in lake BSi, here we show lake BSi is a large terrestrial Al pool due to its high Al content, and lake sedimentary BSi constitutes a significant global sink for Al, which is on the same magnitude as the Al sink in global oceans.

14.
Am J Ophthalmol ; 197: 80-87, 2019 01.
Artículo en Inglés | MEDLINE | ID: mdl-30240726

RESUMEN

PURPOSE: To investigate the primary causes of visual impairment and blindness in rural China. DESIGN: Population-based, cross-sectional study. METHODS: Geographic cluster sampling was used in randomly selecting residents from a rural county/district within 9 provinces in the East Coast, Inland Middle, and West regions of mainland China. Persons aged 50 years or older were enumerated through household visits and invited to examination sites for visual acuity testing and ocular examination. Causes of vision impairment and blindness in 2014 were compared with data from an earlier 2006 survey. RESULTS: Mild visual impairment (20.4% prevalence) was caused by uncorrected refractive error in two thirds of cases and by cataract in nearly another one fourth; moderate-to-severe visual impairment (10.3% prevalence) was caused by cataract in over onec half of cases and by uncorrected refractive error in another one fifth; blindness (1.66% prevalence) was caused by cataract in approximately one half of cases and in another one fourth by retinal disease. Primary causes of visual impairment and blindness in cataract-operated eyes were uncorrected refractive error, posterior capsule opacity, and retinal disease. From 2006 to 2014, the proportion of visual impairment caused by uncorrected refractive error increased, but rates for unoperated cataract were reduced. CONCLUSIONS: Uncorrected refractive error and unoperated cataract are the 2 primary causes of mild, moderate, and severe visual impairment in rural China, with unoperated cataract and retinal diseases primary causes for blindness. An effective public health strategy to increase service delivery for these causes would lead to substantial reduction in vision impairment and blindness.


Asunto(s)
Ceguera/epidemiología , Baja Visión/epidemiología , Anciano , Anciano de 80 o más Años , Catarata/complicaciones , China/epidemiología , Estudios Transversales , Femenino , Humanos , Masculino , Persona de Mediana Edad , Prevalencia , Errores de Refracción/complicaciones , Enfermedades de la Retina/complicaciones , Población Rural/estadística & datos numéricos
15.
Opt Express ; 26(20): 26307-26316, 2018 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-30469720

RESUMEN

Methylammonium lead iodide (CH3NH3PbI3), with the organic-inorganic hybrid perovskite (OIHP) structure, has gained tremendous research interest due to its excellent photo-electron conversion ability in the application of photovoltaics. Despite its solution processed polycrystalline thin film form in solar cells, the single crystalline counterpart may offer some incredibly novel optoelectronic functionalities. In this work, a sizable (>5 mm) and high quality CH3NH3PbI3 single crystal has been synthesized by the inverse temperature crystallization method, and a white-light photodetector of the structure glass/ITO/Ga/ CH3NH3PbI3/Au was fabricated. Overbroad photo-excitation intensities ranging from 0.1 mW/cm2 to 100 mW/cm2 using a sun-light simulator, the on-off ratio is tunable in a wide-range from 65 to 2250 at zero bias voltage. The responsivity (R) and detectivity (D*) are 36.2 mA/W and 2.68×1011 Jones respectively at a weak white-light intensity such as 0.1 mW/cm2. Both the photodetective parameters decrease with the increase of the illumination intensity. Based on impedance spectra obtained at working condition and light intensity dependent Jsc measurements, the surface trap-assist recombination may play a dominating role. The corresponding lifetime (τsurf) and resistance (Rsurf_trap) exhibit fast decays at higher illumination intensities. This fundamental study may pave the way for exploring the contribution of the surface trap-assist recombination in the CH3NH3PbI3 single crystal based photodetector. We believe it is applicable for integration in micro-photonics for sensitive and weak white-light photo-detection.

16.
Molecules ; 22(3)2017 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-28287501

RESUMEN

In this paper, three cationic glycolipids with different hydrophobic chains Malt-DiC12MA (IX a), Malt-DiC14MA (IX b) and Malt-DiC16MA (IX c) were constructed by using maltose as starting material via peracetylation, selective 1-O-deacetylation, trichloroacetimidation, glycosylation, azidation, deacetylation, Staudinger reaction, tertiary amination and quaternization. Target compounds and some intermediates were characterized by ¹H-NMR, 13C-NMR, ¹H-¹H COSY and ¹H-13C HSQC. The results of gel electrophoresis assay, atomic force microscopy images (AFM) and dynamic light scattering (DLS) demonstrate that all the liposomes could efficiently bind and compact DNA (N/P ratio less than 2) into nanoparticles with proper size (88 nm-146 nm, PDI < 0.4) and zeta potential (+15 mV-+26 mV). The transfection efficiency and cellular uptake of glycolipids in HEK293 cell were evaluated through the enhanced green fluorescent protein (EGFP) expression and Cy3-labeled pEGFP-C1 (Enhanced Green Fluorescent Protein plasmid) images, respectively. Importantly, it indicated that Malt-DiC14MA exhibited high gene transfer efficiency and better uptake capability at N/P ratios of 8:1. Additionally, the result of cell viability showed glycolipids exhibited low biotoxicity and good biocompatibility by thiazolyl blue tetrazolium bromide (MTT) assay.


Asunto(s)
Cationes/química , ADN/administración & dosificación , Técnicas de Transferencia de Gen , Liposomas/química , Maltosa/química , Plásmidos/administración & dosificación , Supervivencia Celular , ADN/química , Glucolípidos/química , Células HEK293 , Humanos , Interacciones Hidrofóbicas e Hidrofílicas , Liposomas/síntesis química , Microscopía de Fuerza Atómica , Estructura Molecular , Plásmidos/química , Transfección/métodos
17.
J Colloid Interface Sci ; 461: 64-68, 2016 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-26397911

RESUMEN

The structural incorporation of aluminium (Al) into diatomite is investigated by preparing several Al-diatomite composites by loading an Al precursor, hydroxyl aluminum polymer (Al13), onto the surface of diatomite and heating at various temperatures. The results indicate that Al was incorporated and implanted into the structure of diatomite by the condensation reaction of the hydroxyl groups of Al13 and diatomite, and the Si-O-Al(OH) groups were formed during the condensation reaction. Al incorporation by the condensation reaction of hydroxyl groups of Al13 with single silanols of diatomite occurred more readily than that with geminal silanols. The Al incorporation increased solid acidity of diatomite after Al incorporation. The acidity improvement was various for different types of acid sites, depending on the preparation temperature of the Al-incorporated diatomite. Both Brønsted and Lewis acid sites increased greatly after heating at 250 and 350 °C, but only L acid sites significantly improved after heating at 500 °C. These results demonstrate that the structural incorporation of Al(3+) ions into diatomite can occur by the condensation reaction of the hydroxyl groups of the Al precursors and diatomite. Moreover, the rich solid acid sites of Al-incorporated diatomite show its promising application as a solid acid catalyst.


Asunto(s)
Aluminio/química , Tierra de Diatomeas/química , Hidróxidos/química , Dióxido de Silicio/química , Estructura Molecular , Propiedades de Superficie , Temperatura
18.
J Colloid Interface Sci ; 462: 191-9, 2016 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-26454378

RESUMEN

Hierarchically porous TS-1/modified-diatomite composites with high removal efficiency for methylene blue (MB) were prepared via a facile in situ hydrothermal route. The surface charge state of the diatomite was modified to enhance the electrostatic interactions, followed by in situ hydrothermal coating with TS-1 nanoparticles. The zeolite loading amount in the composites could be adjusted by changing the hydrothermal time. The highest specific surface area and micropore volume of the obtained composites were 521.3m(2)/g and 0.254cm(3)/g, respectively, with an optimized zeolite loading amount of 96.8%. Based on the synergistic effect of efficient adsorption and photocatalysis resulting from the newly formed hierarchically porous structure and improved dispersion of TS-1 nanoparticles onto diatomite, the composites' removal efficiency for MB reached 99.1% after 2h of photocatalytic reaction, even higher than that observed using pure TS-1 nanoparticles. Moreover, the superior MB removal kinetics of the composites were well represented by a pseudo-first-order model, with a rate constant (5.28×10(-2)min(-1)) more than twice as high as that of pure TS-1 nanoparticles (2.43×10(-2)min(-1)). The significant dye removal performance of this novel TS-1/modified-diatomite composite indicates that it is a promising candidate for use in waste water treatment.

19.
J Colloid Interface Sci ; 448: 545-52, 2015 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-25792477

RESUMEN

Naturally occurring porous diatomite (Dt) was functionalized with phenyltriethoxysilane (PTES), and the PTES-modified diatomite (PTES-Dt) was characterized using diffuse reflectance Fourier transform infrared spectroscopy, nitrogen adsorption, nuclear magnetic resonance spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis. After silylation, a functional group (-C6H5, phenyl) was successfully introduced onto the surface of Dt. PTES-Dt exhibited hydrophobic properties with a water contact angle (WCA) as high as 120°±1°, whereas Dt was superhydrophilic with a WCA of 0°. The benzene adsorption data on both Dt and PTES-Dt fit well with the Langmuir isotherm equation. The Langmuir adsorption capacity of benzene on PTES-Dt is 28.1 mg/g, more than 4-fold greater than that on Dt. Moreover, the adsorption kinetics results show that equilibrium was achieved faster for PTES-Dt than for Dt, over the relative pressure range of 0.118-0.157. The excellent benzene adsorption performance of PTES-Dt is attributed to strong π-system interactions between the phenyl groups and the benzene molecules as well as to the macroporosity of the PTES-Dt. These results show that the silylated diatomite could be a new and inexpensive adsorbent suitable for use in benzene emission control.

20.
J Hazard Mater ; 285: 173-81, 2015 Mar 21.
Artículo en Inglés | MEDLINE | ID: mdl-25497031

RESUMEN

Hierarchically porous diatomite/MFI-type zeolite (Dt/Z) composites with excellent benzene adsorption performance were prepared. The hierarchical porosity was generated from the microporous zeolite coated at the surface of diatom frustules and from the macroporous diatomite support. A facile NaOH etching method was employed for the first time to treat the frustule support, followed by hydrothermal growth of MFI-type zeolite at the surface of frustules previously seeded with nanocrystalline silicalite-1 (Sil-1). NaOH etching enlarged the pores on diatom frustules and further increased the coated zeolite contents (W(z)). The central macropore size of the diatom frustules increased from approximately 200-500 nm to 400-1000 nm after NaOH etching. The W(z) could reach 61.2%, while the macroporosity of the composites was largely preserved due to more voids for zeolite coating being formed by NaOH etching. The Dt/Z composites exhibited higher benzene adsorption capacity per unit mass of zeolite and less mass transfer resistance than Sil-1, evaluated via a method of breakthrough curves. These results demonstrate that etching of a diatomite support is a facile but crucial process for the preparation of Dt/Z composites, enabling the resulting composites to become promising candidates for uses in volatile organic compounds emission control.


Asunto(s)
Contaminantes Atmosféricos/química , Benceno/química , Tierra de Diatomeas/química , Hidróxido de Sodio/química , Zeolitas/química , Adsorción , Espectroscopía de Resonancia Magnética , Microscopía Electrónica de Rastreo , Microscopía Electrónica de Transmisión , Difracción de Rayos X
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