Tunable Synthesis of Nitrogen Doped Graphene from Fluorographene under Mild Conditions

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15310%2F20%3A73604116" target="_blank" >RIV/61989592:15310/20:73604116 - isvavai.cz</a>

Výsledek na webu

<a href="https://pubs.acs.org/doi/full/10.1021/acssuschemeng.9b07161" target="_blank" >https://pubs.acs.org/doi/full/10.1021/acssuschemeng.9b07161</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acssuschemeng.9b07161" target="_blank" >10.1021/acssuschemeng.9b07161</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Tunable Synthesis of Nitrogen Doped Graphene from Fluorographene under Mild Conditions

Popis výsledku v původním jazyce

The nitrogen doping of graphene via mild and low energy processes to afford homogeneous product composition and topology with high nitrogen content (&gt;10 at. %) remains a challenge of contemporary 2D materials chemistry. Here, we report a previously unexplored route to synthesize N-doped graphene (NG) with exceptionally high N content (up to 18.2 at. %) by reaction of fluorographene (FG) with NaNH2 in N,N-dimethylformamide (at 130 degrees C) or acetonitrile (at 70 degrees C). The N content can be tuned by changing the reaction time, temperature, and/or solvent, ranging from 6.6 to 18.2 at. %, mainly in the form of pyridinic and pyrrolic configurations. With thermal annealing, the N content remained constant up to 400 degrees C but then decreased by similar to 50% upon being further annealed to 1000 degrees C. Density functional theory (DFT) calculations showed that nitrogen incorporation into the carbon lattice mostly occurred at vacancies present in the starting material. We also conducted a thorough rationalization of side-reaction pathways leading to byproducts, which were confirmed by GC-MS analysis. This is the highest yet recorded N content for a wet chemical doping procedure and at such a low temperature of 70 degrees C. The reported synthetic approach thus offers a sustainable and cost-effective way to prepare NG with a broad tunability window of N content for potential applications related to energy storage and catalysis.

Název v anglickém jazyce

Tunable Synthesis of Nitrogen Doped Graphene from Fluorographene under Mild Conditions

Popis výsledku anglicky

The nitrogen doping of graphene via mild and low energy processes to afford homogeneous product composition and topology with high nitrogen content (&gt;10 at. %) remains a challenge of contemporary 2D materials chemistry. Here, we report a previously unexplored route to synthesize N-doped graphene (NG) with exceptionally high N content (up to 18.2 at. %) by reaction of fluorographene (FG) with NaNH2 in N,N-dimethylformamide (at 130 degrees C) or acetonitrile (at 70 degrees C). The N content can be tuned by changing the reaction time, temperature, and/or solvent, ranging from 6.6 to 18.2 at. %, mainly in the form of pyridinic and pyrrolic configurations. With thermal annealing, the N content remained constant up to 400 degrees C but then decreased by similar to 50% upon being further annealed to 1000 degrees C. Density functional theory (DFT) calculations showed that nitrogen incorporation into the carbon lattice mostly occurred at vacancies present in the starting material. We also conducted a thorough rationalization of side-reaction pathways leading to byproducts, which were confirmed by GC-MS analysis. This is the highest yet recorded N content for a wet chemical doping procedure and at such a low temperature of 70 degrees C. The reported synthetic approach thus offers a sustainable and cost-effective way to prepare NG with a broad tunability window of N content for potential applications related to energy storage and catalysis.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>S - Specificky vyzkum na vysokych skolach

Rok uplatnění

2020

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ACS Sustainable Chemistry &amp; Engineering

ISSN

2168-0485

e-ISSN

—

Svazek periodika

8

Číslo periodika v rámci svazku

12

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

9

Strana od-do

4764-4772

Kód UT WoS článku

000526592900008

EID výsledku v databázi Scopus

2-s2.0-85080960349