Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction

Braga, Adriano H.; Costa, Natália J. S.; Philippot, Karine; Gonçalves, Renato V.; Szanyi, János; Rossi, Liane M.

doi:10.1002/cctc.201902329

Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO₂ reduction

Journal Article · Thu Feb 27 00:00:00 EST 2020 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.201902329· OSTI ID:1843226

^[1]; Costa, Natália J. S. ^[1]; ^[2]; ^[1]; Szanyi, János ^[3]; ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: 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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1843226

Report Number(s):: PNNL-SA-152908

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 11 Vol. 12; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO2 reduction

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Structure and activity of supported bimetallic NiPd nanoparticles: influence of preparation method on CO₂ reduction