Abstract
Highly dispersed low-coordinate Pd sites on SiO2 are fabricated by grafting the PdII PCP-pincer complex (tBuPCP)Pd−OH (tBuPCP = 2,6-C6H3(CH2PtBu2)2) on SiO2, followed by calcination with ozone (100 °C) and reduction with H2 (300 °C). The chemisorption process and structure of this organometallic complex on SiO2 is established by solution-phase1H and31P NMR and solid-state31P CPMAS NMR spectroscopy, XPS, DRIFTS, and AC-HAADF-STEM. The CO adsorption properties of the Pd centers reveal a surprisingly high fraction of adsorption sites where CO is bound in a linear fashion, indicative of low-coordinate Pd. Furthermore, enhanced selectivity of these catalyst centers in aerobic alcohol oxidation versus a control catalyst argues that these low-coordinate sites are the catalytically active sites.
| Original language | English |
|---|---|
| Journal | ACS Catalysis |
| Volume | 6 |
| Issue number | 12 |
| DOIs | |
| Publication status | Published - Jan 1 2016 |
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Keywords
- Benzyl alcohol oxidation
- DRIFTS
- Heterogeneous catalysis
- Palladium nanoparticles
- Solution-phase grafting
- Surface organometallic chemistry
ASJC Scopus subject areas
- Catalysis
Cite this
Direct synthesis of low-Coordinate pd catalysts supported on SiO2 via surface organometallic chemistry. / Liu, Shengsi; Tan, J. Miles; Gulec, Ahmet; Schweitzer, Neil M.; Delferro, Massimiliano; Marks, Laurence D.; Stair, Peter C; Marks, Tobin J.
In: ACS Catalysis, Vol. 6, No. 12, 01.01.2016.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Direct synthesis of low-Coordinate pd catalysts supported on SiO2 via surface organometallic chemistry
AU - Liu, Shengsi
AU - Tan, J. Miles
AU - Gulec, Ahmet
AU - Schweitzer, Neil M.
AU - Delferro, Massimiliano
AU - Marks, Laurence D.
AU - Stair, Peter C
AU - Marks, Tobin J
PY - 2016/1/1
Y1 - 2016/1/1
N2 - Highly dispersed low-coordinate Pd sites on SiO2 are fabricated by grafting the PdII PCP-pincer complex (tBuPCP)Pd−OH (tBuPCP = 2,6-C6H3(CH2PtBu2)2) on SiO2, followed by calcination with ozone (100 °C) and reduction with H2 (300 °C). The chemisorption process and structure of this organometallic complex on SiO2 is established by solution-phase1H and31P NMR and solid-state31P CPMAS NMR spectroscopy, XPS, DRIFTS, and AC-HAADF-STEM. The CO adsorption properties of the Pd centers reveal a surprisingly high fraction of adsorption sites where CO is bound in a linear fashion, indicative of low-coordinate Pd. Furthermore, enhanced selectivity of these catalyst centers in aerobic alcohol oxidation versus a control catalyst argues that these low-coordinate sites are the catalytically active sites.
AB - Highly dispersed low-coordinate Pd sites on SiO2 are fabricated by grafting the PdII PCP-pincer complex (tBuPCP)Pd−OH (tBuPCP = 2,6-C6H3(CH2PtBu2)2) on SiO2, followed by calcination with ozone (100 °C) and reduction with H2 (300 °C). The chemisorption process and structure of this organometallic complex on SiO2 is established by solution-phase1H and31P NMR and solid-state31P CPMAS NMR spectroscopy, XPS, DRIFTS, and AC-HAADF-STEM. The CO adsorption properties of the Pd centers reveal a surprisingly high fraction of adsorption sites where CO is bound in a linear fashion, indicative of low-coordinate Pd. Furthermore, enhanced selectivity of these catalyst centers in aerobic alcohol oxidation versus a control catalyst argues that these low-coordinate sites are the catalytically active sites.
KW - Benzyl alcohol oxidation
KW - DRIFTS
KW - Heterogeneous catalysis
KW - Palladium nanoparticles
KW - Solution-phase grafting
KW - Surface organometallic chemistry
UR - http://www.scopus.com/inward/record.url?scp=85046810481&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85046810481&partnerID=8YFLogxK
U2 - 10.1021/acscatal.6b02046
DO - 10.1021/acscatal.6b02046
M3 - Article
AN - SCOPUS:85046810481
VL - 6
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 12
ER -