Abstract
Selective oxidation of long chain alkanols (+C8+) has deserved much less attention than that of more reactive benzylic or C 1-C4 aliphatic alcohols. Supported gold nanoparticles (NP) are active for the oxidation of alcohols under green chemistry conditions, and high surface supports are used to maximize and stabilize their dispersion. In this work, we investigate hexagonal mesoporous silicas (HMS), pure or modified with metal cations having redox properties (Ce, Fe), as supports of gold NP catalysts for the aerobic oxidation of 1-octanol under green process conditions. Two ways of support modification were used, say, by introducing the modifying cations during the HMS synthesis or by post-synthesis impregnation. Octanal was the main product on every catalyst under the conditions tested (80 C, oxygen flow at atmospheric pressure, solvent base-free heptane); the ester also formed but no acid was detected. Both the composition and the preparation method of the support influenced the activity and stability of the catalysts: the best performance was found on catalysts with post-synthesis impregnated supports, where additional phases of the corresponding oxides are detected by XRD (X-ray diffractometry). IR (infrared) studies of CO adsorption on the catalysts revealed that is due to the different nature of the Au NPs, which are smaller (or positively charged) and preferentially deposited on the modifier oxidic phase in these catalysts.
| Original language | English |
|---|---|
| Pages (from-to) | 65-70 |
| Number of pages | 6 |
| Journal | Catalysis Today |
| Volume | 227 |
| DOIs | |
| Publication status | Published - 15 May 2014 |
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Keywords
- Aerobic oxidation of alcohols
- Gold catalysts
- Gold nanoparticles
- Hexagonal mesoporous silicas
- Octanol oxidation
- Selective oxidation
ASJC Scopus subject areas
- Catalysis
- Chemistry(all)
Cite this
Selective oxidation of 1-octanol over gold supported on mesoporous metal-modified HMS : The effect of the support. / Martínez-González, S.; Gómez-Avilés, A.; Martynyuk, Oxana Anatolievna; Pestryakov, A.; Bogdanchikova, N.; Corberán, V. Cortés.
In: Catalysis Today, Vol. 227, 15.05.2014, p. 65-70.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Selective oxidation of 1-octanol over gold supported on mesoporous metal-modified HMS
T2 - The effect of the support
AU - Martínez-González, S.
AU - Gómez-Avilés, A.
AU - Martynyuk, Oxana Anatolievna
AU - Pestryakov, A.
AU - Bogdanchikova, N.
AU - Corberán, V. Cortés
PY - 2014/5/15
Y1 - 2014/5/15
N2 - Selective oxidation of long chain alkanols (+C8+) has deserved much less attention than that of more reactive benzylic or C 1-C4 aliphatic alcohols. Supported gold nanoparticles (NP) are active for the oxidation of alcohols under green chemistry conditions, and high surface supports are used to maximize and stabilize their dispersion. In this work, we investigate hexagonal mesoporous silicas (HMS), pure or modified with metal cations having redox properties (Ce, Fe), as supports of gold NP catalysts for the aerobic oxidation of 1-octanol under green process conditions. Two ways of support modification were used, say, by introducing the modifying cations during the HMS synthesis or by post-synthesis impregnation. Octanal was the main product on every catalyst under the conditions tested (80 C, oxygen flow at atmospheric pressure, solvent base-free heptane); the ester also formed but no acid was detected. Both the composition and the preparation method of the support influenced the activity and stability of the catalysts: the best performance was found on catalysts with post-synthesis impregnated supports, where additional phases of the corresponding oxides are detected by XRD (X-ray diffractometry). IR (infrared) studies of CO adsorption on the catalysts revealed that is due to the different nature of the Au NPs, which are smaller (or positively charged) and preferentially deposited on the modifier oxidic phase in these catalysts.
AB - Selective oxidation of long chain alkanols (+C8+) has deserved much less attention than that of more reactive benzylic or C 1-C4 aliphatic alcohols. Supported gold nanoparticles (NP) are active for the oxidation of alcohols under green chemistry conditions, and high surface supports are used to maximize and stabilize their dispersion. In this work, we investigate hexagonal mesoporous silicas (HMS), pure or modified with metal cations having redox properties (Ce, Fe), as supports of gold NP catalysts for the aerobic oxidation of 1-octanol under green process conditions. Two ways of support modification were used, say, by introducing the modifying cations during the HMS synthesis or by post-synthesis impregnation. Octanal was the main product on every catalyst under the conditions tested (80 C, oxygen flow at atmospheric pressure, solvent base-free heptane); the ester also formed but no acid was detected. Both the composition and the preparation method of the support influenced the activity and stability of the catalysts: the best performance was found on catalysts with post-synthesis impregnated supports, where additional phases of the corresponding oxides are detected by XRD (X-ray diffractometry). IR (infrared) studies of CO adsorption on the catalysts revealed that is due to the different nature of the Au NPs, which are smaller (or positively charged) and preferentially deposited on the modifier oxidic phase in these catalysts.
KW - Aerobic oxidation of alcohols
KW - Gold catalysts
KW - Gold nanoparticles
KW - Hexagonal mesoporous silicas
KW - Octanol oxidation
KW - Selective oxidation
UR - http://www.scopus.com/inward/record.url?scp=84895492539&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84895492539&partnerID=8YFLogxK
U2 - 10.1016/j.cattod.2013.10.035
DO - 10.1016/j.cattod.2013.10.035
M3 - Article
AN - SCOPUS:84895492539
VL - 227
SP - 65
EP - 70
JO - Catalysis Today
JF - Catalysis Today
SN - 0920-5861
ER -