Co Hydrogenation to Ethanol and Higher Alcohols Over Ultrathin Cucoal Nanosheets Derived from Ldh Precursor

SSRN Electronic Journal(2022)

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摘要
Ultrathin CuCoAl nanosheets derived from layered double hydroxide (LDH) precursor (1-3 cationic-layers) were successfully synthesized by aqueous miscible organic solvent treatment (AMOST) strategy and performed for ethanol and higher alcohols production via CO hydrogenation. The ultrathin CuCoAl nanosheets (CuCo-LDH-aw) demonstrated a comparatively higher total alcohols (ROH) selectivity of 47.6 %, and the molar fraction of ethanol reached up to 37.5 % among the total alcohols. As revealed by XRD, TEM, SEM, BET and AFM char-acterizations, the uniform dispersion of CuCo NPs was observed over the ultrathin CuCoAl nanosheets. Moreover, the optimum ultrathin CuCoAl nanosheets exhibited a higher ratio of Cu+/(Cu0 + Cu+), which exerted a positive role on non-dissociative CO* insertion CHx intermediates. More significantly, XPS and in situ CO-DRIFT tech-niques uncovered the formation of CHx intermediates derived from bridge CO dissociation on the metallic Co species and the formate hydrodeoxygenation route, which involved CO* and surface hydroxyl groups (-OH) reaction. Consequently, it was concluded that the triply synergistic effect of Cu+, Co and surface hydroxyl groups (-OH) species contributed to the improvement in ethanol selectivity via CO hydrogenation.
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关键词
Ultrathin CuCoAl nanosheets, Ethanol, Higher alcohols, CO hydrogenation, Layered double hydroxides
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