Effect of graphene flake size on functionalisation: quantifying reaction extent and imaging locus with single Pt atom tags
Fuente:
Zenodo
Salvato in:
| Autori principali: | , , , , , , |
|---|---|
| Natura: | Recurso digital |
| Pubblicazione: |
Zenodo
2021
|
| Accesso online: | |
| Tags: |
Aggiungi Tag
Nessun Tag, puoi essere il primo ad aggiungerne!!
|
| _version_ | 1866901163141496832 |
|---|---|
| author | Rubio Carrero, Noelia Au, Heather Coulter, Gabriel GUETAZ, Laure GEBEL, Gérard Mattevi, Cecilia Shaffer, Milo |
| author_facet | Rubio Carrero, Noelia Au, Heather Coulter, Gabriel GUETAZ, Laure GEBEL, Gérard Mattevi, Cecilia Shaffer, Milo |
| contents | <p>Here, the locus of functionalisation on graphene-related materials and the progress of the reaction is shown<br>to depend strongly on the starting feedstock. Five characteristically different graphite sources were<br>exfoliated and functionalized using a non-destructive chemical reduction method. These archetypical<br>examples were compared via a model reaction, grafting dodecyl addends, evaluated with TGA-MS, XPS<br>and Raman data. A general increase in grafting ratio (ranging from 1.1 wt% up to 25 wt%) and an<br>improvement in grafting stoichiometry (C/R) were observed as flake radius decreased. Raman spectrum<br>imaging of the functionalised natural flake graphite identified that grafting is directed towards flake<br>edges. This behaviour was further corroborated, at atomistic resolution, by functionalising the graphene<br>layers with bipyridine groups able to complex single platinum atoms. The distribution of these groups<br>was then directly imaged using aberration-corrected HAADF-STEM. Platinum atoms were found to be<br>homogeneously distributed across smaller graphenes; in contrast, a more heterogeneous distribution,<br>with a predominance of edge grafting was observed for larger graphites. These observations show that<br>grafting is directed towards flake edges, but not necessary at edge sites; the mechanism is attributed to<br>the relative inaccessibility of the inner basal plane to reactive moieties, resulting in kinetically driven<br>grafting nearer flake edges. This phenomenology may be relevant to a wide range of reactions on<br>graphenes and other 2d materials.</p> |
| format | Recurso digital |
| id | zenodo_https___doi_org_10_1039_d1sc01958a |
| institution | Zenodo |
| language | |
| publishDate | 2021 |
| publisher | Zenodo |
| record_format | zenodo |
| spellingShingle | Effect of graphene flake size on functionalisation: quantifying reaction extent and imaging locus with single Pt atom tags Rubio Carrero, Noelia Au, Heather Coulter, Gabriel GUETAZ, Laure GEBEL, Gérard Mattevi, Cecilia Shaffer, Milo <p>Here, the locus of functionalisation on graphene-related materials and the progress of the reaction is shown<br>to depend strongly on the starting feedstock. Five characteristically different graphite sources were<br>exfoliated and functionalized using a non-destructive chemical reduction method. These archetypical<br>examples were compared via a model reaction, grafting dodecyl addends, evaluated with TGA-MS, XPS<br>and Raman data. A general increase in grafting ratio (ranging from 1.1 wt% up to 25 wt%) and an<br>improvement in grafting stoichiometry (C/R) were observed as flake radius decreased. Raman spectrum<br>imaging of the functionalised natural flake graphite identified that grafting is directed towards flake<br>edges. This behaviour was further corroborated, at atomistic resolution, by functionalising the graphene<br>layers with bipyridine groups able to complex single platinum atoms. The distribution of these groups<br>was then directly imaged using aberration-corrected HAADF-STEM. Platinum atoms were found to be<br>homogeneously distributed across smaller graphenes; in contrast, a more heterogeneous distribution,<br>with a predominance of edge grafting was observed for larger graphites. These observations show that<br>grafting is directed towards flake edges, but not necessary at edge sites; the mechanism is attributed to<br>the relative inaccessibility of the inner basal plane to reactive moieties, resulting in kinetically driven<br>grafting nearer flake edges. This phenomenology may be relevant to a wide range of reactions on<br>graphenes and other 2d materials.</p> |
| title | Effect of graphene flake size on functionalisation: quantifying reaction extent and imaging locus with single Pt atom tags |
| url | https://doi.org/10.1039/d1sc01958a |