RT Journal Article
T1 Palladium nanoparticles hardwired in carbon nanoreactors enable continually increasing electrocatalytic activity during the hydrogen evolution reaction
A1 Aygün, Mehtap
A1 Guillén Soler, Melanie
A1 Vila Fungueiriño, José Manuel
A1 Chamberlain, Thomas W.
A1 Khlobystov, Andrei N.
A1 Giménez López, María del Carmen
A1 Kurtoglu, Abdullah
K1 Carbon nanoreactors
K1 Electrocatalysis
K1 Hydrogen production
K1 Palladium nanoparticles
K1 Sustainable chemistry
AB Catalysts typically lose effectiveness during operation, with much effort invested in stabilising active metal centres to prolong their functional lifetime for as long as possible. In this study palladium nanoparticles (PdNP) supported inside hollow graphitised carbon nanofibers (GNF), designated as PdNP@GNF, opposed this trend. PdNP@GNF exhibited continuously increasing activity over 30000 reaction cycles when used as an electrocatalyst in the hydrogen evolution reaction (HER). The activity of PdNP@GNF, expressed as the exchange current density, was always higher than activated carbon (Pd/C), and after 10000 cycles PdNP@GNF surpassed the activity of platinum on carbon (Pt/C). The extraordinary durability and self-improving behaviour of PdNP@GNF was solely related the unique nature of the location of the palladium nanoparticles, that is, at the graphitic step-edges within the GNF. Transmission electron microscopy imaging combined with spectroscopic analysis revealed an orchestrated series of reactions occurring at the graphitic step-edges during electrocatalytic cycling, in which some of the curved graphitic surfaces opened up to form a stack of graphene layers bonding directly with Pd atoms through Pd−C bonds. This resulted in the active metal centres becoming effectively hardwired into the electrically conducting nanoreactors (GNF), enabling facile charge transport to/from the catalytic centres resulting in the dramatic self-improving characteristics of the electrocatalyst
PB Wiley
YR 2021
FD 2021
LK http://hdl.handle.net/10347/29063
UL http://hdl.handle.net/10347/29063
LA eng
NO ChemSusChem 2021, 14, 4973.  https://doi.org/10.1002/cssc.202101236
NO This work has received financial support from the Republic of Turkey Ministry of National Education (fellowship for M.A.), the Ministry of Science of Spain (Projects No. RTI2018-101097-A-I00, EIN2019-103246 and RyC-2016-20258 for M.G-L.), the European Research Council (ERC) (Starting Investigator Grant (NANOCOMP-679124) for M.G-L), the Xunta de Galicia (Centro singular de investigación de Galicia accreditation 2016–2019, ED431G/09; convenio colaboracion 2018-AD006), the European Union (European Regional Development Fund – ERDF) and Engineering and Physical Sciences Research Council (EPSRC)
DS Minerva
RD 26 abr 2026