TY - JOUR
T1 - Insight into the efficient oxidation of methyl-ethyl-ketone over hierarchically micro-mesostructured Pt/K-(Al)SiO2 nanorod catalysts
T2 - Structure-activity relationships and mechanism
AU - Jiang, Zeyu
AU - He, Chi
AU - Dummer, Nicholas F.
AU - Shi, Jianwen
AU - Tian, Mingjiao
AU - Ma, Chunyan
AU - Hao, Zhengping
AU - Taylor, Stuart H.
AU - Ma, Mudi
AU - Shen, Zhenxing
N1 - Publisher Copyright:
© 2017 Elsevier B.V.
PY - 2018/6/15
Y1 - 2018/6/15
N2 - Hierarchically micro-mesostructured Pt/K-Al-SiO2 catalysts with regular nanorod (Pt/KA-NRS) and spherical nanoflower-like (Pt/KA-SNFS) morphologies were prepared. The existence of Al atoms generates Brønsted acid sites and reduces silanol groups over the supports, promoting the dispersion of Pt nanoparticles and stability of catalysts. Potassium atoms balance the negative charge of supports and enhance O2 mobility. The Pt/KA-NRS catalysts exhibit unexceptionable low temperature activity, CO2 selectivity, and stability for MEK oxidation. Amongst, 0.27 wt.% Pt/KA-NRS completely converts MEK at just 170 °C (activation energy as low as 37.22 kJ·[rad]mol−1), more than 100 °C lower than other typical Pt/Pd supported catalysts reported in the literature. Diacetyl and 2,3-butandiol are the main intermediates during MEK activation, which convert into H2O and CO2 through aldehydes and acids. The excellent catalytic activity of Pt/KA-NRS is ascribed to their regular morphology, high Pt0 content and dispersion, excellent MEK adsorption capacity and superior O2/CO2 desorption capability under low temperature.
AB - Hierarchically micro-mesostructured Pt/K-Al-SiO2 catalysts with regular nanorod (Pt/KA-NRS) and spherical nanoflower-like (Pt/KA-SNFS) morphologies were prepared. The existence of Al atoms generates Brønsted acid sites and reduces silanol groups over the supports, promoting the dispersion of Pt nanoparticles and stability of catalysts. Potassium atoms balance the negative charge of supports and enhance O2 mobility. The Pt/KA-NRS catalysts exhibit unexceptionable low temperature activity, CO2 selectivity, and stability for MEK oxidation. Amongst, 0.27 wt.% Pt/KA-NRS completely converts MEK at just 170 °C (activation energy as low as 37.22 kJ·[rad]mol−1), more than 100 °C lower than other typical Pt/Pd supported catalysts reported in the literature. Diacetyl and 2,3-butandiol are the main intermediates during MEK activation, which convert into H2O and CO2 through aldehydes and acids. The excellent catalytic activity of Pt/KA-NRS is ascribed to their regular morphology, high Pt0 content and dispersion, excellent MEK adsorption capacity and superior O2/CO2 desorption capability under low temperature.
KW - Activation mechanism
KW - Al-K decorated silica
KW - Catalytic oxidation
KW - Methyl-ethyl-ketone
KW - Monodispersed Pt sites
UR - https://www.scopus.com/pages/publications/85040339398
U2 - 10.1016/j.apcatb.2017.12.007
DO - 10.1016/j.apcatb.2017.12.007
M3 - 文章
AN - SCOPUS:85040339398
SN - 0926-3373
VL - 226
SP - 220
EP - 233
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
ER -