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1.
ACS Appl Mater Interfaces ; 13(43): 51759-51766, 2021 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-34668691

RESUMO

The spatial confinement at metal-zeolite interfaces offers a powerful knob to steer the selectivity of chemical reactions on metal catalysts. However, encapsulating metal catalysts into small-pore zeolites remains a challenging task. Here, we demonstrate an inverse design of metal-zeolite interfaces, "metal-on-zeolite," constructed by area-selective atomic layer deposition. This inverse design bypasses the intrinsic synthetic issues associated with metal encapsulation, offering a potential solution for the fabrication of task-specific metal-zeolite interfaces for desired catalytic applications. Infrared spectroscopy and several probe reactions confirmed the spatial confinement effects at the inverse metal-zeolite interfaces.

2.
Polymers (Basel) ; 12(9)2020 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-32824986

RESUMO

Polysaccharide biopolymers are biomacromolecules derived from renewable resources with versatile functions including thickening, crosslinking, adsorption, etc. Possessing high efficiency and low cost, they have brought wide applications in all phases of petroleum recovery, from well drilling to wastewater treatment. The biopolymers are generally utilized as additives of fluids or plugging agents, to correct the fluid properties that affect the performance and cost of petroleum recovery. This review focuses on both the characteristics of biopolymers and their utilization in the petroleum recovery process. Research on the synthesis and characterization of polymers, as well as controlling their structures through modification, aims to develop novel recipes of biopolymer treatment with new application realms. The influences of biopolymer in many petroleum recovery cases were also evaluated to permit establishing the correlations between their physicochemical properties and performances. As their performance is heavily affected by the local environment, screening and testing polymers under controlled conditions is the necessary step to guarantee the efficiency and safety of biopolymer treatments.

3.
ACS Appl Mater Interfaces ; 12(20): 22778-22788, 2020 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-32338494

RESUMO

Devices driven by above-equilibrium "hot" electrons are appealing for photocatalytic technologies, such as in situ H2O2 synthesis, but currently suffer from low (<1%) overall quantum efficiencies. Gold nanostructures excited by visible light generate hot electrons that can inject into a neighboring semiconductor to drive electrochemical reactions. Here, we designed and studied a metal-insulator-metal (MIM) structure of Au nanoparticles on a ZnO/TiO2/Al film stack, deposited through room-temperature, lithography-free methods. Light absorption, electron injection efficiency, and photocatalytic yield in this device are superior in comparison to the same stack without Al. Our device absorbs >60% of light at the Au localized surface plasmon resonance (LSPR) peak near 530 nm-a 5-fold enhancement in Au absorption due to critical coupling to an Al film. Furthermore, we show through ultrafast pump-probe spectroscopy that the Al-coupled samples exhibit a nearly 5-fold improvement in hot-electron injection efficiency as compared to a non-Al device, with the hot-electron lifetimes extending to >2 ps in devices photoexcited with fluence of 0.1 mJ cm-2. The use of an Al film also enhances the photocatalytic yield of H2O2 more than 3-fold in a visible-light-driven reactor. Altogether, we show that the critical coupling of Al films to Au nanoparticles is a low-cost, lithography-free method for improving visible-light capture, extending hot-carrier lifetimes, and ultimately increasing the rate of in situ H2O2 generation.

4.
Science ; 362(6414): 560-564, 2018 11 02.
Artigo em Inglês | MEDLINE | ID: mdl-30385572

RESUMO

The synthesis of ultrasmall supported bimetallic nanoparticles (between 1 and 3 nanometers in diameter) with well-defined stoichiometry and intimacy between constituent metals remains a substantial challenge. We synthesized 10 different supported bimetallic nanoparticles via surface inorganometallic chemistry by decomposing and reducing surface-adsorbed heterometallic double complex salts, which are readily obtained upon sequential adsorption of target cations and anions on a silica substrate. For example, adsorption of tetraamminepalladium(II) [Pd(NH3)4 2+] followed by adsorption of tetrachloroplatinate [PtCl4 2-] was used to form palladium-platinum (Pd-Pt) nanoparticles. These supported bimetallic nanoparticles show enhanced catalytic performance in acetylene selective hydrogenation, which clearly demonstrates a synergistic effect between constituent metals.

5.
Artigo em Inglês | MEDLINE | ID: mdl-29664220

RESUMO

Double network (DN) hydrogels, a kind of promising soft and tough hydrogels, are produced by two unique contrasting networks with designed network entanglement burst into the field of materials science as versatile functional systems for a very broad range of applications. A part of the DN hydrogels is characterized by extraordinary mechanical properties providing efficient biocompatible and high strength for holding considerable promise in tissue engineering. Following DN hydrogels principles and consideration of biomedical applications, we provide an overall view of the present various DN hydrogels and look forward to the future of DN hydrogels for tissue engineering. In this review, the preparation methods, structure, properties, current situation, and challenges are mainly discussed for the purpose of tissue engineering. This article is categorized under: Implantable Materials and Surgical Technologies > Nanomaterials and Implants Implantable Materials and Surgical Technologies > Nanotechnology in Tissue Repair and Replacement.


Assuntos
Materiais Biocompatíveis/química , Hidrogéis/química , Engenharia Tecidual/métodos , Animais , Materiais Biocompatíveis/síntese química , Fenômenos Biomecânicos , Reagentes de Ligações Cruzadas , Humanos , Hidrogéis/síntese química , Teste de Materiais , Nanotecnologia , Próteses e Implantes , Engenharia Tecidual/tendências , Alicerces Teciduais/química
6.
Sci Total Environ ; 634: 141-149, 2018 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-29627536

RESUMO

A series of Mo2N/HZSM-5 and transition metal modified Mo2N/HZSM-5 catalysts were prepared for the catalytic upgrading of pine wood-derived pyrolytic vapors for the selective production of monocyclic aromatic hydrocarbons (MAHs), while restraining the formation of polycyclic aromatic hydrocarbons (PAHs). Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to determine the effects of several factors on selective MAHs production, including Mo2N loading on HZSM-5, transition metal (Fe, Ce, La, Cu, Cr) modification of Mo2N/HZSM-5, pyrolysis temperature, and catalyst-to-biomass ratio. In addition, quantitative experiments were conducted to determine the actual yields of major aromatic hydrocarbons and the source of aromatic hydrocarbons from basic biomass components. Results indicated that among the various catalysts, the Ce-10%Mo2N/HZSM-5 exhibited the best performance on promoting the formation of MAHs and restraining the generation of PAHs. Under the optimal conditions, the actual yields of MAHs and PAHs from Ce-10%Mo2N/HZSM-5 catalytic process were 99.8mg/g and 7.5mg/g, while those from HZSM catalyst were only 77.2mg/g and 23.7mg/g respectively. Furthermore, the possible catalytic mechanism of the Ce-Mo2N/HZSM-5 catalyst was proposed based on the catalyst characterization.

7.
Materials (Basel) ; 11(4)2018 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-29570658

RESUMO

CeO2 is a promising catalytic oxidation material for flue gas mercury removal. Density functional theory (DFT) calculations and periodic slab models are employed to investigate mercury adsorption and oxidation by oxygen over the CeO2 (111) surface. DFT calculations indicate that Hg° is physically adsorbed on the CeO2 (111) surface and the Hg atom interacts strongly with the surface Ce atom according to the partial density of states (PDOS) analysis, whereas, HgO is adsorbed on the CeO2 (111) surface in a chemisorption manner, with its adsorption energy in the range of 69.9-198.37 kJ/mol. Depending on the adsorption methods of Hg° and HgO, three reaction pathways (pathways I, II, and III) of Hg° oxidation by oxygen are proposed. Pathway I is the most likely oxidation route on the CeO2 (111) surface due to it having the lowest energy barrier of 20.7 kJ/mol. The formation of the HgO molecule is the rate-determining step, which is also the only energy barrier of the entire process. Compared with energy barriers of Hg° oxidation on the other catalytic materials, CeO2 is more efficient at mercury removal in flue gas owing to its low energy barrier.

8.
ACS Omega ; 3(7): 8421-8428, 2018 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-31458970

RESUMO

Electricity generation from coal, nuclear reaction, and shale gas has brought environmental, safety, and health concerns. The electricity industry is constantly seeking sustainable, safe, and healthy way of electricity generation. The use of triboelectric device is promising for producing electricity from water energy. In this study, we report on the rapid fabrication of a 1,3-phosphorylated poly(vinyl alcohol) gel-based triboelectric device and direct harvesting of water turbulence energy using this device. The gel was prepared by the reaction of poly(vinyl alcohol) with dipotassium phosphate. The synthesized gel was characterized by mass spectroscopy, thermogravimetric analysis/difference thermogravimetry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscope, Raman, and carbon and oxygen K-edges soft X-ray absorption near edge structure spectroscopy. The triboelectric device was used to harvest electricity from water turbulence.

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