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1.
Heliyon ; 10(12): e32894, 2024 Jun 30.
Article in English | MEDLINE | ID: mdl-38994084

ABSTRACT

This study investigated the novel application of Fe-TiO2-allophane catalysts with 6.0 % w/w of iron oxide and two TiO2 proportions (10 % and 30 % w/w) for degrading atrazine (ATZ) using the heterogeneous dual-effect (HDE) process under sunlight. Comparative analyses with Fe-allophane and TiO2-allophane catalysts were conducted in both photocatalysis (PC) and HDE processes. FTIR spectra reveal the unique hydrous feldspathoids structure of allophane, showing evidence of new bond formation between Si-O groups of allophane clays and iron hydroxyl species, as well as Si-O-Ti bonds that intensified with higher TiO2 content. The catalysts exhibited an anatase structure. In Fe-TiO2-allophane catalysts, iron oxide was incorporated through the substitution of Ti4+ by Fe3+ in the anatase crystal lattice and precipitation on the surface of allophane clays, forming small iron oxide particles. Allophane clays reduced the agglomeration and particle size of TiO2, resulting in an enhanced specific surface area and pore volume for all catalysts. Iron oxide incorporation decreased the band gap, broadening the photoresponse to visible light. In the PC process, TiO2-allophane achieves 90 % ATZ degradation, attributed to radical species from the UV component of sunlight. In the HDE process, Fe-TiO2-allophane catalysts exhibit synergistic effects, particularly with 30 % w/w TiO2, achieving 100 % ATZ degradation and 85 % COD removal, with shorter reaction time as TiO2 percentage increased. The HDE process was performed under less acidic conditions, achieving complete ATZ degradation after 6 h without iron leaching. Consequently, Fe-TiO2-allophane catalysts are proposed as a promising alternative for degrading emerging pollutants under environmentally friendly conditions.

2.
Nanomaterials (Basel) ; 12(7)2022 Mar 23.
Article in English | MEDLINE | ID: mdl-35407166

ABSTRACT

The synthesis of methanol by carbon dioxide hydrogenation has been studied using copper-molybdenum carbides supported on high surface area graphite, reduced graphene oxide and carbon nanotubes. The synthesis conditions and the effect of the support were studied. The catalysts were prepared in situ using H2 or He at 600 °C or 700 °C. Both molybdenum carbide and oxycarbide were obtained. A support with less reactive carbon resulted in lower proportion of carbide obtained. The best results were achieved over a 5 wt.% Cu and 10 wt.% Mo on high surface area graphite that reached 96.3% selectivity to methanol.

3.
Nanomaterials (Basel) ; 10(11)2020 Nov 04.
Article in English | MEDLINE | ID: mdl-33158119

ABSTRACT

Nickel-cobalt bimetallic catalysts supported on high surface area graphite with different Ni:Co ratios (3:1, 2:1 and 1:1) and the monometallic Ni and Co were prepared by wetness impregnation method. The catalysts were tested in hydrodeoxygenation (HDO) of guaiacol in the liquid phase at 50 bar of H2 and 300 °C. The materials were characterized by N2 adsorption-desorption, XRD, TEM/STEM, H2-TPR, and CO-chemisorption to assess their properties and correlate them with the catalytic results. The activity was higher on the bimetallic catalysts and followed the trend NiCo2:1/G ∼ NiCo3:1/G > NiCo1:1/G > Co/G > Ni/G. Also, selectivity results showed that Ni was more active in the hydrogenation favoring cyclohexanol production from phenol, while this was inhibited on the Co-containing catalysts. Hence, the results showed that synergy was created between Ni and Co and that their interaction, properties, and catalytic performance depend on the metals' ratio.

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