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1.
ACS Omega ; 8(1): 1643-1651, 2023 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-36643468

RESUMO

Heat distribution and good adhesion of the washcoat on monolith catalysts are critical to improving catalytic activity and long-term stability. Compared with cordierite, metal foam presents a high thermal conductivity coefficient. Also, the availability of "washcoat" in situ grown on metal substrates opens the door to eliminating the problem of coating peeling. Generally, hydrothermal or thermal methods are used for the fabrication of in situ grown washcoat on metal substrates. In this research, the aluminum foam monolith vertically aligned Al2O3 nanowire array is successfully prepared at ambient temperature in an alkaline solution for the first time. Furthermore, the Pt-loaded Al2O3 nanowire array (0.5 gPt/L monolith) is applied to C2H4 degradation. The catalyst converts 90% C2H4 at 147 °C with a gas hourly space velocity (GHSV) of 20,000 h-1. And a little decrease (1%) is observed in catalytic activity, even in 15 vol % water vapors. The catalysts show good thermal stability and water resistance property over 36 h at 300 °C. Above all, this study presents a simple way of in situ growth of washcoat on metal-substrate monolith with potentially scaled manufacturing. And the monolith catalyst shows good catalytic performance on C2H4, which can be applied for volatile organic compound treatment.

2.
Front Chem ; 10: 1085035, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36451928

RESUMO

[This corrects the article DOI: 10.3389/fchem.2022.978698.].

3.
Front Chem ; 10: 978698, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36082198

RESUMO

Pd/Al2O3 catalysts modified by different chemical elements (Mg, Si, Ce, and Zr) were tested for methane (CH4) catalytic combustion, and PdO nanoparticles loaded on modified Al2O3 were systematically studied. These conditions assess the carrier effects of Pd/Al2O3 and acid strength influences on CH4 combustion. We observed carrier effects on activation energy through tuning Pd 3d binding energies (BEs) and on pre-exponential factors (A) through Pd dispersion and acidity on supports. When the BE of Pd 3d5/2 is 337.3 eV, PdO nanoparticles loaded on modified Al2O3 have excellent activity in cracking the C-H bond of CH4, which leads to the lowest activation energy (E a ), regardless of the size effect of the PdO nanoparticle. Furthermore, a theoretical construction that acid sites on catalysts promote the reversible elementary step (2Pd-OH ↔ Pd-O* + Pd* + H2O) right shifts improving the A dependency on the quantity of exposed Pd* and Pd-O*. As a result, Al2O3, as the carrier, not only modifies the electronic characteristics and size of supported PdO nanoparticles but also participates in the reaction process via acid sites on the surface of Al2O3.

4.
Chemistry ; 24(9): 2126-2136, 2018 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-28857303

RESUMO

We present a general and facile synthesis strategy, on the basis of metal-ammine complex chemistry, for synthesizing hollow transition-metal oxides (Co3 O4 , NiO, CuO-Cu2 O, and ZnO)/nitrogen-doped graphene hybrids, potentially applied in high-performance lithium-ion batteries. The oxygen-containing functional groups of graphene oxide play a prerequisite role in the formation of hollow transition-metal oxides on graphene nanosheets, and a significant hollowing process occurs only when forming metal (Co2+ , Ni2+ , Cu2+ , or Zn2+ )-ammine complex ions. Moreover, the hollowing process is well correlated with the complexing capacity between metal ions and NH3 molecules. The significant hollowing process occurs for strong metal-ammine complex ions including Co2+ , Ni2+ , Cu2+ , and Zn2+ ions, and no hollow structures formed for weak and/or noncomplex Mn2+ and Fe3+ ions. Simultaneously, this novel strategy can also achieve the direct doping of nitrogen atoms into the graphene framework. The electrochemical performance of two typical hollow Co3 O4 or NiO/nitrogen-doped graphene hybrids was evaluated by their use as anodic materials. It was demonstrated that these unique nanostructured hybrids, in contrast with the bare counterparts, solid transition-metal oxides/nitrogen-doped graphene hybrids, perform with significantly improved specific capacity, superior rate capability, and excellent capacity retention.

5.
J Colloid Interface Sci ; 513: 903-910, 2018 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-29278856

RESUMO

Mercaptans are highly volatile compounds responsible for disagreeable odors and very low olfactory threshold, especially for CH3SH (0.4 ppvb). To the best knowledge of us, approach for controlling low-concentrated odors (i.e. 1-10 ppm) is scarcely reported. In this research, Cu-doped mesoporous silica was synthesized for removal of low-concentrated CH3SH. The as-prepared samples show considerably thermal and mechanical stability and could be thermal-regenerated. Copper loading ratio and humidity have significant impacts on eliminating odors. According to XRD, TEM, BET, NMR and EPR, we deduce that surface groups on CuO nanoparticles and the SiOCu group are highly possibly transformed into a hydrated complex which is much more effective in capturing CH3SH with its empty Cu-3d orbit. Although CH3SH has to compete with water for absorption sites, it is always the "winner" owing to the strong chelating ability between SH group and Cu (Ⅱ).

6.
Nanoscale ; 8(34): 15763-73, 2016 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-27531821

RESUMO

A hierarchical CoCo layered double hydroxide (LDH) nanostructure was constructed through a facile topochemical transformation route under a dynamic oxygen atmosphere. Self-assembled coral-like CoAl LDH nanostructures via the homogeneous precipitation method were also inspected under different ammonia-releasing reagents and solvents. Benzene and toluene were chosen as probe molecules to evaluate their catalytic performance over the metal oxide CoCoO and CoAlO calcined from their corresponding LDH precursors. Nanocatalyst of trivalent Co ions replaced Al(3+) ions in the bruited-like layer had a higher catalytic activity (T99(benzene) = 210 °C and T99(toluene) = 220 °C at a space velocity = 60 000 mL g(-1) h(-1)). Raman spectroscopy, XPS and H2-TPR demonstrated the existence of abundant high valence Co ions that serve as active sites. TPD verified the types of active oxygen species and surface acid properties. It was concluded that the high valence Co ions induced excellent low-temperature reducibility. Surface Lewis acid sites and the surface Oads/Olatt molar ratio (0.61) played relevant roles in determining its catalytic oxidation performance. Our design in this work provides a promising approach for the development of nanocatalysts with exposed desirable defects.

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