dc.contributor.author | Lunney, James | en |
dc.contributor.author | Perova, Tatiana | en |
dc.contributor.author | Colavita, Paula | en |
dc.date.accessioned | 2021-02-23T12:40:34Z | |
dc.date.available | 2021-02-23T12:40:34Z | |
dc.date.issued | 2020 | en |
dc.date.submitted | 2020 | en |
dc.identifier.citation | Hoque, M.K. and Behan, J.A. and Creel, J. and Lunney, J.G. and Perova, T.S. and Colavita, P.E., Reactive Plasma N-Doping of Amorphous Carbon Electrodes: Decoupling Disorder and Chemical Effects on Capacitive and Electrocatalytic Performance, Frontiers in Chemistry, 8, 2020 | en |
dc.identifier.other | Y | en |
dc.description | PUBLISHED | en |
dc.description | cited By 0 | en |
dc.description.abstract | Nitrogen-free amorphous carbon thin films prepared via sputtering followed by graphitization, were used as precursor materials for the creation of N-doped carbon electrodes with varying degrees of amorphization. Incorporation of N-sites was achieved via nitrogen plasma treatments which resulted in both surface functionalization and amorphization of the carbon electrode materials. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were used to monitor composition and carbon organization: results indicate incorporation of predominantly pyrrolic-N sites after relatively short treatment cycles (5 min or less), accompanied by an initial etching of amorphous regions followed by a slower process of amorphization of graphitized clusters. By leveraging the difference in the rate of these two processes it was possible to investigate the effects of chemical N-sites and C-defect sites on their electrochemical response. The materials were tested as metal-free electrocatalysts in the oxygen reduction reaction (ORR) in alkaline conditions. We find that the introduction of predominantly pyrrolic-N sites via plasma modification results in improvements in selectivity in the ORR, relative to the nitrogen-free precursor material. Introduction of defects through prolonged plasma exposure has a more pronounced and beneficial effect on ORR descriptors than introduction of N-sites alone, leading to both increased onset potentials, and reduced hydroperoxide yields relative to the nitrogen-free carbon material. Our results suggest that increased structural disorder/heterogeneity results in the introduction of carbon sites that might either serve as main activity sites, or that enhance the effects of N-functionalities in the ORR via synergistic effects. | en |
dc.language.iso | en | en |
dc.relation.ispartofseries | Frontiers in Chemistry | en |
dc.relation.ispartofseries | 8 | en |
dc.relation.uri | doi: 10.3389/fchem.2020.593932 | en |
dc.rights | Y | en |
dc.subject | ORR via synergistic effects | en |
dc.subject | Nitrogen-free amorphous carbon thin films | en |
dc.subject | graphitization | en |
dc.subject | Amorphous Carbon (a-C) | en |
dc.subject | Carbon | en |
dc.subject | Electrocatalysis and functionalized/modified electrodes | en |
dc.subject | Metal-free | en |
dc.subject | Nitrogen plasma (nitridation) | en |
dc.subject | Nitrogen plasma activation | en |
dc.title | Reactive Plasma N-Doping of Amorphous Carbon Electrodes: Decoupling Disorder and Chemical Effects on Capacitive and Electrocatalytic Performance | en |
dc.type | Journal Article | en |
dc.type.supercollection | scholarly_publications | en |
dc.type.supercollection | refereed_publications | en |
dc.identifier.peoplefinderurl | http://people.tcd.ie/jlunney | en |
dc.identifier.peoplefinderurl | http://people.tcd.ie/perovat | en |
dc.identifier.peoplefinderurl | http://people.tcd.ie/colavitp | en |
dc.identifier.rssinternalid | 224312 | en |
dc.identifier.doi | http://dx.doi.org/10.3389/fchem.2020.593932 | en |
dc.rights.ecaccessrights | openAccess | |
dc.relation.cites | Cites | en |
dc.subject.TCDTheme | Nanoscience & Materials | en |
dc.subject.TCDTag | Electrochemistry | en |
dc.identifier.orcid_id | 0000-0003-3430-5198 | en |
dc.status.accessible | N | en |
dc.contributor.sponsor | Irish Research Council (IRC) | en |
dc.contributor.sponsorGrantNumber | GOIPG/2014/399. | en |
dc.contributor.sponsor | Science Foundation Ireland (SFI) | en |
dc.contributor.sponsorGrantNumber | 13/CDA/2213. | en |
dc.identifier.uri | http://hdl.handle.net/2262/95309 | |