Abstract
Palladium nanoparticles (Pd NPs) supported on organoamine-functionalized SBA-15 mesoporous silica are known to have higher catalytic activity for formic acid dehydrogenation than Pd NPs supported on plain, unmodified SBA-15 mesoporous silica. The organoamine groups present around the Pd NPs play important roles in stabilizing the Pd NPs, providing strong metal-molecular support interaction (SMMSI) to the Pd NPs, and rendering enhanced catalytic activities to the materials toward formic acid dehydrogenation. However, detailed studies on the effects of different types of amine groups on the catalytic activities of mesoporous silica-supported Pd NPs toward formic acid dehydrogenation have not been reported. Herein, we describe the synthesis of SBA-15 mesoporous silica grafted with three types of organoamine groups (primary, secondary, and tertiary amine), which are further decorated with tetraamminepalladium(ii) complexes that are then reduced to Pd NPs in situ with 10% of H2/N2 at 250 °C. The effects of the different compositional and steric properties associated with the amine groups on (i) the electronic properties of the Pd NPs, (ii) the size of the Pd NPs, and (iii) the structure-property relationships of the materials were closely examined. Based on the results, the materials' catalytic activities toward dehydrogenation of formic acid to generate hydrogen (H2) for fuel cells were determined.
| Original language | English |
|---|---|
| Pages (from-to) | 16150-16161 |
| Number of pages | 12 |
| Journal | Journal of Materials Chemistry A |
| Volume | 5 |
| Issue number | 31 |
| DOIs | |
| Publication status | Published - Jan 1 2017 |
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ASJC Scopus subject areas
- Chemistry(all)
- Renewable Energy, Sustainability and the Environment
- Materials Science(all)
Cite this
Formic acid dehydrogenation over Pd NPs supported on amine-functionalized SBA-15 catalysts : Structure-activity relationships. / Koh, Katherine; Jeon, Mina; Yoon, Chang Won; Asefa, Teddy.
In: Journal of Materials Chemistry A, Vol. 5, No. 31, 01.01.2017, p. 16150-16161.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Formic acid dehydrogenation over Pd NPs supported on amine-functionalized SBA-15 catalysts
T2 - Structure-activity relationships
AU - Koh, Katherine
AU - Jeon, Mina
AU - Yoon, Chang Won
AU - Asefa, Teddy
PY - 2017/1/1
Y1 - 2017/1/1
N2 - Palladium nanoparticles (Pd NPs) supported on organoamine-functionalized SBA-15 mesoporous silica are known to have higher catalytic activity for formic acid dehydrogenation than Pd NPs supported on plain, unmodified SBA-15 mesoporous silica. The organoamine groups present around the Pd NPs play important roles in stabilizing the Pd NPs, providing strong metal-molecular support interaction (SMMSI) to the Pd NPs, and rendering enhanced catalytic activities to the materials toward formic acid dehydrogenation. However, detailed studies on the effects of different types of amine groups on the catalytic activities of mesoporous silica-supported Pd NPs toward formic acid dehydrogenation have not been reported. Herein, we describe the synthesis of SBA-15 mesoporous silica grafted with three types of organoamine groups (primary, secondary, and tertiary amine), which are further decorated with tetraamminepalladium(ii) complexes that are then reduced to Pd NPs in situ with 10% of H2/N2 at 250 °C. The effects of the different compositional and steric properties associated with the amine groups on (i) the electronic properties of the Pd NPs, (ii) the size of the Pd NPs, and (iii) the structure-property relationships of the materials were closely examined. Based on the results, the materials' catalytic activities toward dehydrogenation of formic acid to generate hydrogen (H2) for fuel cells were determined.
AB - Palladium nanoparticles (Pd NPs) supported on organoamine-functionalized SBA-15 mesoporous silica are known to have higher catalytic activity for formic acid dehydrogenation than Pd NPs supported on plain, unmodified SBA-15 mesoporous silica. The organoamine groups present around the Pd NPs play important roles in stabilizing the Pd NPs, providing strong metal-molecular support interaction (SMMSI) to the Pd NPs, and rendering enhanced catalytic activities to the materials toward formic acid dehydrogenation. However, detailed studies on the effects of different types of amine groups on the catalytic activities of mesoporous silica-supported Pd NPs toward formic acid dehydrogenation have not been reported. Herein, we describe the synthesis of SBA-15 mesoporous silica grafted with three types of organoamine groups (primary, secondary, and tertiary amine), which are further decorated with tetraamminepalladium(ii) complexes that are then reduced to Pd NPs in situ with 10% of H2/N2 at 250 °C. The effects of the different compositional and steric properties associated with the amine groups on (i) the electronic properties of the Pd NPs, (ii) the size of the Pd NPs, and (iii) the structure-property relationships of the materials were closely examined. Based on the results, the materials' catalytic activities toward dehydrogenation of formic acid to generate hydrogen (H2) for fuel cells were determined.
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U2 - 10.1039/c7ta02040f
DO - 10.1039/c7ta02040f
M3 - Article
VL - 5
SP - 16150
EP - 16161
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 31
ER -