Abstract
Single atoms and few-atom clusters of platinum are uniformly installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and X-ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.
| Original language | English |
|---|---|
| Pages (from-to) | 909-913 |
| Number of pages | 5 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 57 |
| Issue number | 4 |
| DOIs | |
| Publication status | Published - Jan 22 2018 |
Fingerprint
Keywords
- atomic layer deposition (ALD)
- heterogeneous catalysis
- metal–organic frameworks (MOFs)
- platinum
- sinter-resistance
ASJC Scopus subject areas
- Catalysis
- Chemistry(all)
Cite this
Sinter-Resistant Platinum Catalyst Supported by Metal–Organic Framework. / Kim, In Soo; Li, Zhanyong; Zheng, Jian; Platero-Prats, Ana E.; Mavrandonakis, Andreas; Pellizzeri, Steven; Ferrandon, Magali; Vjunov, Aleksei; Gallington, Leighanne C.; Webber, Thomas E.; Vermeulen, Nicolaas A.; Penn, R. Lee; Getman, Rachel B.; Cramer, Christopher J.; Chapman, Karena W.; Camaioni, Donald M.; Fulton, John L.; Lercher, Johannes A.; Farha, Omar K.; Hupp, Joseph T; Martinson, Alex B.F.
In: Angewandte Chemie - International Edition, Vol. 57, No. 4, 22.01.2018, p. 909-913.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Sinter-Resistant Platinum Catalyst Supported by Metal–Organic Framework
AU - Kim, In Soo
AU - Li, Zhanyong
AU - Zheng, Jian
AU - Platero-Prats, Ana E.
AU - Mavrandonakis, Andreas
AU - Pellizzeri, Steven
AU - Ferrandon, Magali
AU - Vjunov, Aleksei
AU - Gallington, Leighanne C.
AU - Webber, Thomas E.
AU - Vermeulen, Nicolaas A.
AU - Penn, R. Lee
AU - Getman, Rachel B.
AU - Cramer, Christopher J.
AU - Chapman, Karena W.
AU - Camaioni, Donald M.
AU - Fulton, John L.
AU - Lercher, Johannes A.
AU - Farha, Omar K.
AU - Hupp, Joseph T
AU - Martinson, Alex B.F.
PY - 2018/1/22
Y1 - 2018/1/22
N2 - Single atoms and few-atom clusters of platinum are uniformly installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and X-ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.
AB - Single atoms and few-atom clusters of platinum are uniformly installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 °C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and X-ray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. These results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.
KW - atomic layer deposition (ALD)
KW - heterogeneous catalysis
KW - metal–organic frameworks (MOFs)
KW - platinum
KW - sinter-resistance
UR - http://www.scopus.com/inward/record.url?scp=85039761733&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85039761733&partnerID=8YFLogxK
U2 - 10.1002/anie.201708092
DO - 10.1002/anie.201708092
M3 - Article
VL - 57
SP - 909
EP - 913
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 4
ER -