Open Access
JACS Au, volume 1, issue 4, pages 450-458
Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation
Scott R Docherty
1
,
Nat Phongprueksathat
2
,
Erwin Lam
1
,
Gina Noh
1
,
Olga V. Safonova
3
,
Atsushi Urakawa
2
,
Publication type: Journal Article
Publication date: 2021-03-17
General Medicine
Abstract
The direct conversion of CO2 to CH3OH represents an appealing strategy for the mitigation of anthropogenic CO2 emissions. Here, we report that small, narrowly distributed alloyed PdGa nanoparticles, prepared via surface organometallic chemistry from silica-supported GaIII isolated sites, selectively catalyze the hydrogenation of CO2 to CH3OH. At 230 °C and 25 bar, high activity (22.3 molMeOH molPd-1 h-1) and selectivity for CH3OH/DME (81%) are observed, while the corresponding silica-supported Pd nanoparticles show low activity and selectivity. X-ray absorption spectroscopy (XAS), IR, NMR, and scanning transmission electron microscopy-energy-dispersive X-ray provide evidence for alloying in the as-synthesized material. In situ XAS reveals that there is a dynamic dealloying/realloying process, through Ga redox, while operando diffuse reflectance infrared Fourier transform spectroscopy demonstrates that, while both methoxy and formate species are observed in reaction conditions, the relative concentrations are inversely proportional, as the chemical potential of the gas phase is modulated. High CH3OH selectivities, across a broad range of conversions, are observed, showing that CO formation is suppressed for this catalyst, in contrast to reported Pd catalysts.
Top-30
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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1 publication, 2.7%
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Citations by publishers
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American Chemical Society (ACS)
17 publications, 45.95%
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Wiley
5 publications, 13.51%
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Elsevier
4 publications, 10.81%
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Royal Society of Chemistry (RSC)
4 publications, 10.81%
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Springer Nature
2 publications, 5.41%
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The Chemical Society of Japan
1 publication, 2.7%
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Multidisciplinary Digital Publishing Institute (MDPI)
1 publication, 2.7%
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Taylor & Francis
1 publication, 2.7%
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Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii
1 publication, 2.7%
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- We do not take into account publications without a DOI.
- Statistics recalculated only for publications connected to researchers, organizations and labs registered on the platform.
- Statistics recalculated weekly.
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Docherty S. R. et al. Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation // JACS Au. 2021. Vol. 1. No. 4. pp. 450-458.
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Docherty S. R., Phongprueksathat N., Lam E., Noh G., Safonova O. V., Urakawa A., Copéret C. Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation // JACS Au. 2021. Vol. 1. No. 4. pp. 450-458.
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TY - JOUR
DO - 10.1021/jacsau.1c00021
UR - https://doi.org/10.1021/jacsau.1c00021
TI - Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation
T2 - JACS Au
AU - Docherty, Scott R
AU - Phongprueksathat, Nat
AU - Noh, Gina
AU - Safonova, Olga V.
AU - Urakawa, Atsushi
AU - Copéret, Christophe
AU - Lam, Erwin
PY - 2021
DA - 2021/03/17 00:00:00
PB - American Chemical Society (ACS)
SP - 450-458
IS - 4
VL - 1
SN - 2691-3704
SN - 2691-3704
ER -
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@article{2021_Docherty,
author = {Scott R Docherty and Nat Phongprueksathat and Gina Noh and Olga V. Safonova and Atsushi Urakawa and Christophe Copéret and Erwin Lam},
title = {Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation},
journal = {JACS Au},
year = {2021},
volume = {1},
publisher = {American Chemical Society (ACS)},
month = {mar},
url = {https://doi.org/10.1021/jacsau.1c00021},
number = {4},
pages = {450--458},
doi = {10.1021/jacsau.1c00021}
}
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MLA
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Docherty, Scott R., et al. “Silica-Supported PdGa Nanoparticles: Metal Synergy for Highly Active and Selective CO2-to-CH3OH Hydrogenation.” JACS Au, vol. 1, no. 4, Mar. 2021, pp. 450-458. https://doi.org/10.1021/jacsau.1c00021.