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1.
ACS Appl Mater Interfaces ; 15(38): 44887-44898, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37721481

RESUMO

Supported palladium (Pd) catalysts are widely utilized to reduce the emission of exhaust CH4 from lean-burn engines by catalytic combustion. A large amount of water vapor in the exhaust makes hydroxyls accumulate on the catalyst surface at temperatures below 450 °C, leading to severe catalyst deactivation. Tuning palladium chemistry and inhibiting water adsorption are critical to developing active catalysts. Modifying the support surface with inert silicates would both change the palladium-support interaction and decrease water adsorption sites. This study reports an improved Pd/Y2O3-ZrO2 catalyst by constructing silicate patches on yttria-stabilized zirconia (Y2O3-ZrO2) support. The silicates hindered electron transfer from Y2O3-ZrO2 oxygen vacancies to palladium, which optimized palladium chemistry, especially the reducibility of active PdO species, and thereby boosted CH4 conversion under dry conditions. The temperature of 90% methane conversion (T90) over the catalyst decreased from 386 to 309 °C. Moreover, the inert silicates decreased surface oxygen vacancies of Y2O3-ZrO2 to improve support hydrophobicity, thereby inhibiting hydroxyl accumulation. The poisoning effect of water on the active sites located on the palladium-silicate interface was alleviated. When reaction gases contained 10 vol % water, the silicate-modified catalyst still showed higher activity with T90 of 404 °C, which is lower than T90 of 452 °C for unmodified catalyst. This work represents a step forward in preparing high-performance palladium catalysts for low-temperature wet methane combustion.

2.
Nanomaterials (Basel) ; 11(12)2021 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-34947778

RESUMO

Non-platinum carbon-based catalysts have attracted much more attention in recent years because of their low cost and outstanding performance, and are regarded as one of the most promising alternatives to precious metal catalysts. Activated carbon (AC), which has a large specific surface area (SSA), can be used as a carrier or carbon source at the same time. In this work, stable pine peel bio-based materials were used to prepare large-surface-area activated carbon and then compound with cobalt phthalocyanine (CoPc) to obtain a high-performance cobalt/nitrogen/carbon (Co-N-C) catalyst. High catalytic activity is related to increasing the number of Co particles on the large-specific-area activated carbon, which are related with the immersing effect of CoPc into the AC and the rational decomposed temperature of the CoPc ring. The synergy with N promoting the exposure of CoNx active sites is also important. The Eonset of the catalyst treated with a composite proportion of AC and CoPc of 1 to 2 at 800 °C (AC@CoPc-800-1-2) is 1.006 V, higher than the Pt/C (20 wt%) catalyst. Apart from this, compared with other AC/CoPc series catalysts and Pt/C (20 wt%) catalyst, the stability of AC/CoPc-800-1-2 is 87.8% in 0.1 M KOH after 20,000 s testing. Considering the performance and price of the catalyst in a practical application, these composite catalysts combining biomass carbon materials with phthalocyanine series could be widely used in the area of catalysts and energy storage.

3.
Chemistry ; 27(58): 14478-14488, 2021 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-34331494

RESUMO

MnCo2 O4 is derived from a Co/Mn bimetallic metal-organic framework (MOF). Then Ni-MOF is directly grown on the surface of the obtained MnCo2 O4 to form a nano-flower structure with small balls. A large surface area, abundant active sites of MnCo2 O4 and porosity of Ni-MOF allow the prepared MnCo2 O4 /Ni-MOF composite material to deliver an excellent electrochemical performance. At the same time, an appropriate thermal treatment temperature of the MnCo2 O4 precursor is also very important for controlling the morphology of the obtained MnCo2 O4 and electrochemical performances of the resulted composite material including electric conductivity, specific capacitance and rate performance. The prepared MnCo2 O4 -600/Ni-MOF shows an ultrahigh rate performance (when the current density increases from 1 to 10 A g-1 , the capacitance retention rate is as high as 93.41 %) and good cycle stability (the assembled asymmetric supercapacitor advice delivers a capacitance retention rate of 94.74 % after 20 000 charge and discharge cycles) as well as a relatively high specific capacitance. These excellent electrochemical properties indicate that MnCo2 O4 /Ni-MOF has a good application prospect in the market.

4.
ACS Appl Mater Interfaces ; 8(51): 35545-35551, 2016 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-27966871

RESUMO

Overvoltage protection is becoming increasingly important because of miniaturization and multifunctionality of electronic devices. Flexible, easily processable materials with nonlinear and reversible I-V behavior are highly desired. In this study, hybrid nanoparticles of ZnO-decorated carbon nanotubes (CNT-ZnO) were synthesized via a sol-gel hydrothermal process employed in an epoxy matrix to prepare composites. Microstructure analysis demonstrated that ZnO nanoparticles were well-bonded to the surface of CNT. The CNT-ZnO/epoxy composites exhibited nonlinear I-V behavior under increasingly applied voltage with a nonlinear coefficient of 5.01 (10 wt % filler loading). More importantly, the composites possessed excellent reversibility from dielectric to conductor and vise versa in the recycling of increase and decrease of applied electric field, in contrast to the poor recoverability of pure CNT-filled epoxy. The mechanism of the nonlinear I-V behavior and reversibility was investigated and discussed. A simple circuit was fabricated, which verified well the protection function of the CNT-ZnO/polymer composites.

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