TY - JOUR
T1 - Ru-based nanoparticles supported on carbon nanotubes for electrocatalytic hydrogen evolution
T2 - structural and electronic effects
AU - Romero, Nuria
AU - Fenoll, Dídac A.
AU - Gil, Laia
AU - Campos, Sergi
AU - Creus, Jordi
AU - Martí, Gerard
AU - Heras-Domingo, Javier
AU - Collière, Vincent
AU - Mesa, Camilo A.
AU - Giménez, Sixto
AU - Francàs, Laia
AU - Rodríguez-Santiago, Luis
AU - Solans-Monfort, Xavier
AU - Sodupe, Mariona
AU - Bofill, Roger
AU - Philippot, Karine
AU - García-Antón, Jordi
AU - Sala, Xavier
N1 - Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2023/10/10
Y1 - 2023/10/10
N2 - The performance of Ru-based nanoparticles (NPs) in the hydrogen evolution reaction (HER) relies on both their structural properties and the oxidation state of the metal. Herein, the versatility of the organometallic approach for the synthesis of metal-based nanostructures is combined with thermal oxidation treatments to prepare carbon-nanotube (CNT)-supported Ru-containing nanomaterials for their use as electrocatalysts after dropcasting onto a glassy carbon rotating disk electrode. This strategy allowed access to a series of hybrid nanomaterials of different Ru/RuO2 compositions and different structural order. Linear sweep voltammetry experiments show that the relative disposition of the Ru/RuO2 phases, their interconversion under reductive turnover conditions and the degree of structural order affect the HER electrocatalytic performance of different materials. The electrode containing NPs consisting of a RuO2 core and metallic Ru at the surface outperforms that containing either pure RuO2 NPs or Ru NPs. Impedance spectroscopy studies and DFT calculations suggest that this catalytic activity enhancement arises from improved charge transport properties and from the structure of the exposed metallic Ru shell, which is partially oxidized and highly amorphous.
AB - The performance of Ru-based nanoparticles (NPs) in the hydrogen evolution reaction (HER) relies on both their structural properties and the oxidation state of the metal. Herein, the versatility of the organometallic approach for the synthesis of metal-based nanostructures is combined with thermal oxidation treatments to prepare carbon-nanotube (CNT)-supported Ru-containing nanomaterials for their use as electrocatalysts after dropcasting onto a glassy carbon rotating disk electrode. This strategy allowed access to a series of hybrid nanomaterials of different Ru/RuO2 compositions and different structural order. Linear sweep voltammetry experiments show that the relative disposition of the Ru/RuO2 phases, their interconversion under reductive turnover conditions and the degree of structural order affect the HER electrocatalytic performance of different materials. The electrode containing NPs consisting of a RuO2 core and metallic Ru at the surface outperforms that containing either pure RuO2 NPs or Ru NPs. Impedance spectroscopy studies and DFT calculations suggest that this catalytic activity enhancement arises from improved charge transport properties and from the structure of the exposed metallic Ru shell, which is partially oxidized and highly amorphous.
KW - Catalytic-activity
KW - Ruthenium nanoparticles
UR - http://www.scopus.com/inward/record.url?scp=85165354594&partnerID=8YFLogxK
UR - https://www.mendeley.com/catalogue/c72f08f5-9847-3906-aa1f-0c3c4888085e/
U2 - 10.1039/d3qi00698k
DO - 10.1039/d3qi00698k
M3 - Article
AN - SCOPUS:85165354594
SN - 2052-1545
VL - 10
SP - 5885
EP - 5896
JO - Inorganic Chemistry Frontiers
JF - Inorganic Chemistry Frontiers
IS - 20
ER -