Unveiling the formation mechanism of PbxPdy intermetallic phases in solvothermal synthesis using in situ X-ray total scattering
Borup, Anders Bæk ; Bertelsen, Andreas Dueholm ; Kløve, Magnus ; Christensen, Rasmus Stubkjær ; Broge, Nils Lau Nyborg ; Dippel, Ann Christin ; Jørgensen, Mads Ry Vogel LU
and Iversen, Bo Brummerstedt
(2023)
In Nanoscale
15(45).
p.18481-18488
- Abstract
Pd possesses attractive catalytic properties and nano-structuring is an obvious way to enhance catalytic activity. Alloying Pd with Pb has been shown to enhance the catalytic effect of alcohol oxidation. Further optimization of the catalytic effect can be accomplished by controlling the particle size and key to this is understanding the formation mechanism. By monitoring solvothermal syntheses using in situ X-ray total scattering, this study unveils the formation mechanism of PbxPdy intermetallic nanoparticles. The formation occurs through a multi-step mechanism. Initially, Pd nanoparticles are formed, followed by incorporation of Pb into the Pd-structure, thus forming PbxPdy intermetallic... (More)
Pd possesses attractive catalytic properties and nano-structuring is an obvious way to enhance catalytic activity. Alloying Pd with Pb has been shown to enhance the catalytic effect of alcohol oxidation. Further optimization of the catalytic effect can be accomplished by controlling the particle size and key to this is understanding the formation mechanism. By monitoring solvothermal syntheses using in situ X-ray total scattering, this study unveils the formation mechanism of PbxPdy intermetallic nanoparticles. The formation occurs through a multi-step mechanism. Initially, Pd nanoparticles are formed, followed by incorporation of Pb into the Pd-structure, thus forming PbxPdy intermetallic nanoparticles. By varying the reaction time and temperature, the incorporation of Pb can be controlled, thereby tailoring the phase outcome. Based on the in situ solvothermal syntheses, ex situ autoclave syntheses were performed, resulting in the synthesis of Pb3Pd5 and Pb9Pd13 with a purity above 93%. The catalytic effect of these intermetallic phases towards the hydrogen evolution reaction (HER) is assessed. It is found that Pd, Pb3Pd5, and Pb9Pd13 have comparable stabilities, however, the overpotential increases with increasing amounts of Pb.
(Less)
- author
- Borup, Anders Bæk
; Bertelsen, Andreas Dueholm
; Kløve, Magnus
; Christensen, Rasmus Stubkjær
; Broge, Nils Lau Nyborg
; Dippel, Ann Christin
; Jørgensen, Mads Ry Vogel
LU
and Iversen, Bo Brummerstedt
- organization
- publishing date
- 2023-11-01
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Nanoscale
- volume
- 15
- issue
- 45
- pages
- 8 pages
- publisher
- Royal Society of Chemistry
- external identifiers
-
- pmid:37942507
- scopus:85176815391
- ISSN
- 2040-3364
- DOI
- 10.1039/d3nr03901c
- language
- English
- LU publication?
- yes
- additional info
- Publisher Copyright: © 2023 The Royal Society of Chemistry.
- id
- d1d5fa9a-63e9-46b8-8190-724b68e980bb
- date added to LUP
- 2024-01-11 09:57:36
- date last changed
- 2024-04-26 05:41:36
@article{d1d5fa9a-63e9-46b8-8190-724b68e980bb,
abstract = {{<p>Pd possesses attractive catalytic properties and nano-structuring is an obvious way to enhance catalytic activity. Alloying Pd with Pb has been shown to enhance the catalytic effect of alcohol oxidation. Further optimization of the catalytic effect can be accomplished by controlling the particle size and key to this is understanding the formation mechanism. By monitoring solvothermal syntheses using in situ X-ray total scattering, this study unveils the formation mechanism of Pb<sub>x</sub>Pd<sub>y</sub> intermetallic nanoparticles. The formation occurs through a multi-step mechanism. Initially, Pd nanoparticles are formed, followed by incorporation of Pb into the Pd-structure, thus forming Pb<sub>x</sub>Pd<sub>y</sub> intermetallic nanoparticles. By varying the reaction time and temperature, the incorporation of Pb can be controlled, thereby tailoring the phase outcome. Based on the in situ solvothermal syntheses, ex situ autoclave syntheses were performed, resulting in the synthesis of Pb<sub>3</sub>Pd<sub>5</sub> and Pb<sub>9</sub>Pd<sub>13</sub> with a purity above 93%. The catalytic effect of these intermetallic phases towards the hydrogen evolution reaction (HER) is assessed. It is found that Pd, Pb<sub>3</sub>Pd<sub>5</sub>, and Pb<sub>9</sub>Pd<sub>13</sub> have comparable stabilities, however, the overpotential increases with increasing amounts of Pb.</p>}},
author = {{Borup, Anders Bæk and Bertelsen, Andreas Dueholm and Kløve, Magnus and Christensen, Rasmus Stubkjær and Broge, Nils Lau Nyborg and Dippel, Ann Christin and Jørgensen, Mads Ry Vogel and Iversen, Bo Brummerstedt}},
issn = {{2040-3364}},
language = {{eng}},
month = {{11}},
number = {{45}},
pages = {{18481--18488}},
publisher = {{Royal Society of Chemistry}},
series = {{Nanoscale}},
title = {{Unveiling the formation mechanism of Pb<sub>x</sub>Pd<sub>y</sub> intermetallic phases in solvothermal synthesis using in situ X-ray total scattering}},
url = {{http://dx.doi.org/10.1039/d3nr03901c}},
doi = {{10.1039/d3nr03901c}},
volume = {{15}},
year = {{2023}},
}