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1.
Sci Total Environ ; 830: 154818, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35341871

RESUMO

Under the background of indoor air formaldehyde decontamination, a freestanding ultra-light assembly was fabricated via ice-templating approach starting from MnO2 nanoparticles and environmentally benign agar powder. The 3D composite of agar and MnO2 (AM-3D) was comparatively studied with powdered counterparts (including pure MnO2 and mixture of agar and MnO2) and the 3D-structured agar for formaldehyde oxidation, and their physicochemical properties were examined with XRD, ATR, SEM, XPS, isothermal N2 adsorption, ESR, Raman, CO-TPR and O2-TPD. For the single test of formaldehyde oxidation, the AM-3D catalyst exhibited 62.0%-67.0% removal percentage for ~400 mg/m3 formaldehyde, which did not demonstrate significant advantage over the control samples. However, thanks to the porous 3D agar scaffold with large spatial volume that could promote a rapid gas-phase formaldehyde concentration reduction, and the strong interaction between the dispersed MnO2 particles and agar substrate that could afford a large amount of reactive oxygen species to further oxidize the adsorbed formaldehyde, the AM-3D composite was a much better HCHO-to-CO2 converter and possessed much more advantageous stability for repeated cycles of formaldehyde oxidation: even after ten cycles, there was still 41.7% of formaldehyde removed. Furthermore, the viable sunlight irradiation could easily restore the activity of the used AM-3D catalyst back to the level approaching that of the fresh one. Finally, reaction pathways were put forward via the infrared spectroscopic and ion chromatographic investigations on the surface intermediates of the spent materials.


Assuntos
Compostos de Manganês , Óxidos , Ágar , Catálise , Formaldeído , Compostos de Manganês/química , Oxirredução , Óxidos/química , Oxigênio/química
2.
J Phys Chem Lett ; 12(50): 12062-12066, 2021 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-34908416

RESUMO

The electrodissolution of Au(111) in anaerobic cupric/ammonia/thiosulfate solutions, typical of a non-equilibrium dissipative system, was investigated via in situ electrochemical atomic force microscopy. At a specific initial concentration ratio of aqueous ammonia to cupric ions, the pit number and average pit area increase autocatalytically, while the pit depth increases monotonically during dissolution. A further increase in this initial concentration ratio leads to oscillatory dynamics in the pit number and average pit area while the pit depth fluctuates between one and two atoms. Mechanistic analysis indicates that alternation between formation and dissolution of a sulfur film results in periodic pitting, which produces gold dissolution layer by layer. This work presents a new dissolution mode, i.e., periodic layer dissolution generated by oscillatory pitting processes in addition to a pitting mode with a continually increasing depth, and the use of high initial concentration ratios of ammonia to cupric ion to accelerate the elimination of passivating sulfur film for Au dissolution.

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