Low-temperature CO oxidation over Ag/SiO2 catalysts: Effect of OH/Ag ratio

被引:94
|
作者
Dutov, V. V. [1 ]
Mamontov, G. V. [1 ]
Zaikovskii, V. I. [2 ,3 ]
Liotta, L. F. [4 ]
Vodyankina, O. V. [1 ]
机构
[1] Tomsk State Univ, 36 Lenina Ave, Tomsk, Russia
[2] Boreskov Inst Catalysis, 5 Lavrentiev Ave, Novosibirsk, Russia
[3] Novosibirsk State Univ, 2 Pirogova St, Novosibirsk, Russia
[4] CNR, Inst Nanostruct Mat ISMN, Via Ugo La Malfa 153, Palermo, Italy
关键词
CO oxidation; Silver nanoparticles; Silica surface; OH/Ag ratio; SUPPORTED SILVER CATALYSTS; CARBON-MONOXIDE OXIDATION; SELECTIVE OXIDATION; AG NANOPARTICLES; AG/AL-SBA-15; CATALYSTS; OXYGEN-ADSORPTION; SILICA; PRETREATMENT; AG/SBA-15; SURFACE;
D O I
10.1016/j.apcatb.2017.09.051
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
Combined application of TPx methods, H-2-O-2 titration, UV-vis DRS, TGA-DSC-MS, TEM, XRD, N-2 adsorption at -196 degrees C allowed proving the OH/Ag molar ratio as the key parameter defining the catalytic properties of silica-supported silver (Ag/SiO2) in low-temperature CO oxidation. A new insight into the. formation of active species on the catalyst surface is presented. In this study, Ag/SiO2 catalysts with Ag loading of 5 and 8 wt.% were prepared by incipient wetness impregnation method on the basis of commercial silicas preliminary calcined at 500, 700 and 900 degrees C. Detailed characterization of catalysts by physicochemical methods revealed that molar ratio between the concentration of surface OH groups (normalized to support mass) and silver amount in the prepared catalysts (OH/Ag ratio) affects the silver dispersion, structure of silver nanoparticles (NPs) and their catalytic properties. Only at optimal value of OH/Ag ratio the silver NPs are stated to possess both high dispersion and defective multidomain structure (that consists of several nanodomains) providing the adsorption of weakly bound oxygen species responsible for high catalytic activity in CO oxidation at low -temperature. Additionally, the co-existence of two types of active sites reacting with CO at room temperature with and without formation of adsorbed carbonate species is discussed. The first type of active sites was catalytically active in low-temperature CO oxidation with CO2 release at room temperature (RT). The second type may retain surface carbonate species up to similar to 40-50 degrees C. The balance between these species shifts towards the first type for the active catalyst.
引用
收藏
页码:598 / 609
页数:12
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