Insight into the efficient oxidation of methyl-ethyl-ketone over hierarchically micro-mesostructured Pt/K-(Al)SiO2 nanorod catalysts: Structure-activity relationships and mechanism

被引:76
作者
Jiang, Zeyu [1 ]
He, Chi [1 ,2 ]
Dummer, Nicholas F. [2 ]
Shi, Jianwen [3 ]
Tian, Mingjiao [1 ]
Ma, Chunyan [4 ]
Hao, Zhengping [4 ]
Taylor, Stuart H. [2 ]
Ma, Mudi [1 ]
Shen, Zhenxing [1 ]
机构
[1] Xi An Jiao Tong Univ, Dept Environm Sci & Engn, State Key Lab Multiphase Flow Power Engn, Sch Energy & Power Engn, Xian 710049, Shaanxi, Peoples R China
[2] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg Pk Pl, Cardiff CF10 3AT, S Glam, Wales
[3] Xi An Jiao Tong Univ, Ctr Nanomat Renewable Energy, State Key Lab Elect Insulat & Power Equipment, Sch Elect Engn, Xian 710049, Shaanxi, Peoples R China
[4] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Dept Environm Nanomat, Beijing 100085, Peoples R China
基金
中国国家自然科学基金;
关键词
Monodispersed Pt sites; Al-K decorated silica; Methyl-ethyl-ketone; Catalytic oxidation; Activation mechanism; VOLATILE ORGANIC-COMPOUNDS; IN-SITU FTIR; ROOM-TEMPERATURE; SURFACE-PROPERTIES; PT/TIO2; CATALYSTS; CO OXIDATION; NOBLE-METALS; NANOPARTICLES; FORMALDEHYDE; PERFORMANCE;
D O I
10.1016/j.apcatb.2017.12.007
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 Bronsted 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 O-2 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 degrees C (activation energy as low as 37.22 kJ.mol(-1)), more than 100 degrees 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 Pt content and dispersion, excellent MEK adsorption capacity and superior O-2/CO2 desorption capability under low temperature.
引用
收藏
页码:220 / 233
页数:14
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