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Tuning Cu+ species/Brønsted acids of copper phyllosilicate by K+ doping for selective hydrogenation of methyl palmitate to hexadecanol
(2023-12-01)
Prasanseang, Warot
;
Choojun, Kittisak
;
Poo-arporn, Yingyot
;
Huang, Ai Lin
;
Lin, Yu Chuan
Selective hydrogenation of methyl palmitate to hexadecanol can be manipulated by tuning Cu+ species and Brønsted acid sites (BAS) of copper phyllosilicate (CuPS) catalysts with K+ doping. The catalysts were prepared by impregnating K+ onto reduced and non-reduced CuPS. The reactions were carried out in a fixed-bed flow reactor at 250 °C under atmospheric H<inf>2</inf>. In situ TR-XANES and Py-IR suggest that the presence of K+ could stabilize Cu+ species and neutralize BAS. As compared to the non-reduced sample, K+ loading (0.01–0.10 wt%) on the reduced CuPS provide higher Cu+ fraction (10–16%), lower BAS (0.82 to 0.16μ mol/g) and lower Cu dispersion (75 to 52%). A balance between Cu0 active surface and Cu+ content provides an optimum hydrogenation activity (up to 80 %). The increased Cu+ species, together with the decreased BAS, does not only enhance the catalyst stability, but also hexadecanol selectivity (from 35 to 60%, at ∼50% conversion).
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Linear long-chain α-olefins from hydrodeoxygenation of methyl palmitate over copper phyllosilicate catalysts
(2022-04-05)
Prasanseang, Warot
;
Choojun, Kittisak
;
Poo-arporn, Yingyot
;
Huang, Ai Lin
;
Lin, Yu Chuan
Copper phyllosilicate (CuPS) was used as a bifunctional catalyst for hydrodeoxygenation of methyl palmitate (MP) to produce long-chain α-olefins without the loss of carbon backbone. The CuPS catalysts were prepared by ammonia evaporation-hydrothermal method. The crystal structure, surface area, reducibility, Cu dispersion, Cu particle size and acidity of the catalysts were examined by XRD, BET, H<inf>2</inf>-TPR, TEM, NH<inf>3</inf>-TPD and Py-IR. The existence of Cu2+ species (octahedral (O<inf>h</inf>)/square planar (Sq)), Cu+ and Cu0 upon calcination/reduction was investigated by in situ TR-XANES. The Cu dispersion was related to the Cu+ fraction in CuPS, while Brønsted acid sites (BAS) depends on Cu0 particles. The MP conversion to 1-hexadecene proceeds via hydrogenation-dehydration promoted by the synergy of Cu0 surface and Brønsted acid sites at the interface. The α-olefin selectivity depends on a balance between Cu+ and Cu loading. The 20CuPS possessing 10% Cu+ fraction, provides a high conversion of 72% with 45% α-olefin selectivity.

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