Abstract
Herein, we describe a strategy for converting catalytically inactive, highly crystalline nanoparticle superlattices embedded in silica into catalytically active, porous structures through superlattice assembly and calcination. First, a body-centered cubic (bcc) superlattice is synthesized through the assembly of two sets of 5 nm gold nanoparticles chemically modified with DNA bearing complementary sticky end sequences. These superlattices are embedded in silica and calcined at 350 °C to provide access to the catalytic nanoparticle surface sites. The calcined superlattice maintains its bcc ordering and has a surface area of 210 m2/g. The loading of catalytically active nanoparticles within the superlattice was determined by inductively coupled plasma mass spectrometry, which revealed that the calcined superlattice contained approximately 10% Au by weight. We subsequently investigate the ability of supported Au nanoparticle superlattices to catalyze alcohol oxidation. In addition to demonstrating that calcined superlattices are effective catalysts for alcohol oxidation, electron microscopy reveals preservation of the crystalline structure of the bcc superlattice following calcination and catalysis. Unlike many bulk nanoparticle catalysts, which are difficult to characterize and susceptible to aggregation, nanoparticle superlattices synthesized using DNA interactions offer an attractive bottom-up route to structurally defined heterogeneous catalysts, where one has the potential to independently control nanoparticle size, nanoparticle compositions, and interparticle spacings.
| Original language | English |
|---|---|
| Pages (from-to) | 1658-1662 |
| Number of pages | 5 |
| Journal | Journal of the American Chemical Society |
| Volume | 137 |
| Issue number | 4 |
| DOIs | |
| Publication status | Published - Feb 4 2015 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
- Medicine(all)
Cite this
Controlling structure and porosity in catalytic nanoparticle superlattices with DNA. / Auyeung, Evelyn; Morris, William; Mondloch, Joseph E.; Hupp, Joseph T; Farha, Omar K.; Mirkin, Chad A.
In: Journal of the American Chemical Society, Vol. 137, No. 4, 04.02.2015, p. 1658-1662.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Controlling structure and porosity in catalytic nanoparticle superlattices with DNA
AU - Auyeung, Evelyn
AU - Morris, William
AU - Mondloch, Joseph E.
AU - Hupp, Joseph T
AU - Farha, Omar K.
AU - Mirkin, Chad A.
PY - 2015/2/4
Y1 - 2015/2/4
N2 - Herein, we describe a strategy for converting catalytically inactive, highly crystalline nanoparticle superlattices embedded in silica into catalytically active, porous structures through superlattice assembly and calcination. First, a body-centered cubic (bcc) superlattice is synthesized through the assembly of two sets of 5 nm gold nanoparticles chemically modified with DNA bearing complementary sticky end sequences. These superlattices are embedded in silica and calcined at 350 °C to provide access to the catalytic nanoparticle surface sites. The calcined superlattice maintains its bcc ordering and has a surface area of 210 m2/g. The loading of catalytically active nanoparticles within the superlattice was determined by inductively coupled plasma mass spectrometry, which revealed that the calcined superlattice contained approximately 10% Au by weight. We subsequently investigate the ability of supported Au nanoparticle superlattices to catalyze alcohol oxidation. In addition to demonstrating that calcined superlattices are effective catalysts for alcohol oxidation, electron microscopy reveals preservation of the crystalline structure of the bcc superlattice following calcination and catalysis. Unlike many bulk nanoparticle catalysts, which are difficult to characterize and susceptible to aggregation, nanoparticle superlattices synthesized using DNA interactions offer an attractive bottom-up route to structurally defined heterogeneous catalysts, where one has the potential to independently control nanoparticle size, nanoparticle compositions, and interparticle spacings.
AB - Herein, we describe a strategy for converting catalytically inactive, highly crystalline nanoparticle superlattices embedded in silica into catalytically active, porous structures through superlattice assembly and calcination. First, a body-centered cubic (bcc) superlattice is synthesized through the assembly of two sets of 5 nm gold nanoparticles chemically modified with DNA bearing complementary sticky end sequences. These superlattices are embedded in silica and calcined at 350 °C to provide access to the catalytic nanoparticle surface sites. The calcined superlattice maintains its bcc ordering and has a surface area of 210 m2/g. The loading of catalytically active nanoparticles within the superlattice was determined by inductively coupled plasma mass spectrometry, which revealed that the calcined superlattice contained approximately 10% Au by weight. We subsequently investigate the ability of supported Au nanoparticle superlattices to catalyze alcohol oxidation. In addition to demonstrating that calcined superlattices are effective catalysts for alcohol oxidation, electron microscopy reveals preservation of the crystalline structure of the bcc superlattice following calcination and catalysis. Unlike many bulk nanoparticle catalysts, which are difficult to characterize and susceptible to aggregation, nanoparticle superlattices synthesized using DNA interactions offer an attractive bottom-up route to structurally defined heterogeneous catalysts, where one has the potential to independently control nanoparticle size, nanoparticle compositions, and interparticle spacings.
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U2 - 10.1021/ja512116p
DO - 10.1021/ja512116p
M3 - Article
C2 - 25611764
AN - SCOPUS:84922423538
VL - 137
SP - 1658
EP - 1662
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 4
ER -