Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction
Abstract
Here, bimetallic Ni-Pd and monometallic reference catalysts were prepared by decomposing organometallic precursors, Ni(cod)2 and Pd2(dba)3, leading to nanoparticles with sizes ranging from 3 to 6 nm. Two different synthesis procedures were followed: i) solution synthesis using capping ligand (hexadecylamine) followed by impregnation of pre-formed nanoparticles on SiO2, called Sol-immobilization (SI); and 2) direct precursor decomposition onto SiO2, without stabilizer, called Direct Decomposition (DD). Samples prepared by SI procedure are alloyed bimetallic nanoparticles, whereas samples obtained by DD one show phase segregation. Interestingly, DD samples show better activity for CO2 hydrogenation into CO (reverse water-gas shift reaction - RWGS) than SI ones. The best compromise between activity for CO2 activation (at lower temperature) and CO selectivity was achieved with Ni DD and NiPd DD catalysts. Moreover, the addition of palladium increased the concentration of surface undercoordinated sites, which chemisorb CO weakly, thus improving activity and selectivity, in opposition to other samples that chemisorb CO strongly, in multiband configuration. In the presence of Pd, different decomposition rates drive the formation of smaller and more active Ni clusters. The knowledge acquired here on the influence of synthesis conditions on the catalytic properties of Ni-Pd catalysts should guide us to better catalysts formore »
- Authors:
-
[1];
[2];
[1];
[1]
- Univ. of Sao Paulo (Brazil)
- Centre National de la Recherche Scientifique (CNRS) (France); Laboratoire de Chimie de Coordination (LCC) (France); Univ. of Toulouse (France)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Org.:
- Fundação de Amparo a Pesquisa do Estado de São Paulo (FAPESP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1843226
- Report Number(s):
- PNNL-SA-152908
Journal ID: ISSN 1867-3880
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 11; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bimetallic nanoparticles; CO2 hydrogenation; Segregation; alloy; activity
Citation Formats
Braga, Adriano H., Costa, Natália J. S., Philippot, Karine, Gonçalves, Renato V., Szanyi, János, and Rossi, Liane M. Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction. United States: N. p., 2020.
Web. doi:10.1002/cctc.201902329.
Braga, Adriano H., Costa, Natália J. S., Philippot, Karine, Gonçalves, Renato V., Szanyi, János, & Rossi, Liane M. Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction. United States. https://doi.org/10.1002/cctc.201902329
Braga, Adriano H., Costa, Natália J. S., Philippot, Karine, Gonçalves, Renato V., Szanyi, János, and Rossi, Liane M. Thu .
"Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction". United States. https://doi.org/10.1002/cctc.201902329. https://www.osti.gov/servlets/purl/1843226.
@article{osti_1843226,
title = {Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction},
author = {Braga, Adriano H. and Costa, Natália J. S. and Philippot, Karine and Gonçalves, Renato V. and Szanyi, János and Rossi, Liane M.},
abstractNote = {Here, bimetallic Ni-Pd and monometallic reference catalysts were prepared by decomposing organometallic precursors, Ni(cod)2 and Pd2(dba)3, leading to nanoparticles with sizes ranging from 3 to 6 nm. Two different synthesis procedures were followed: i) solution synthesis using capping ligand (hexadecylamine) followed by impregnation of pre-formed nanoparticles on SiO2, called Sol-immobilization (SI); and 2) direct precursor decomposition onto SiO2, without stabilizer, called Direct Decomposition (DD). Samples prepared by SI procedure are alloyed bimetallic nanoparticles, whereas samples obtained by DD one show phase segregation. Interestingly, DD samples show better activity for CO2 hydrogenation into CO (reverse water-gas shift reaction - RWGS) than SI ones. The best compromise between activity for CO2 activation (at lower temperature) and CO selectivity was achieved with Ni DD and NiPd DD catalysts. Moreover, the addition of palladium increased the concentration of surface undercoordinated sites, which chemisorb CO weakly, thus improving activity and selectivity, in opposition to other samples that chemisorb CO strongly, in multiband configuration. In the presence of Pd, different decomposition rates drive the formation of smaller and more active Ni clusters. The knowledge acquired here on the influence of synthesis conditions on the catalytic properties of Ni-Pd catalysts should guide us to better catalysts for CO2 transformations into valuable products.},
doi = {10.1002/cctc.201902329},
journal = {ChemCatChem},
number = 11,
volume = 12,
place = {United States},
year = {Thu Feb 27 00:00:00 EST 2020},
month = {Thu Feb 27 00:00:00 EST 2020}
}
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