Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems

Ulises Martinez, Joseph H. Dumont, Edward F. Holby, Kateryna Artyushkova, Geraldine M. Purdy, Akhilesh Singh, Nathan H. Mack, Plamen Atanassov, David A. Cullen, Karren L. More, Manish Chhowalla, Piotr Zelenay, Andrew M. Dattelbaum, Aditya D. Mohite, Gautam Gupta

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

Graphitic materials are essential in energy conversion and storage because of their excellent chemical and electrical properties. The strategy for obtaining functional graphitic materials involves graphite oxidation and subsequent dissolution in aqueous media, forming graphene-oxide nanosheets (GNs). Restacked GNs contain substantial intercalated water that can react with heteroatom dopants or the graphene lattice during reduction. We demonstrate that removal of intercalated water using simple solvent treatments causes significant structural reorganization, substantially affecting the oxygen reduction reaction (ORR) activity and stability of nitrogen-doped graphitic systems. Amid contrasting reports describing the ORR activity of GN-based catalysts in alkaline electrolytes, we demonstrate superior activity in an acidic electrolyte with an onset potential of ~0.9 V, a half-wave potential (E ½) of 0.71 V, and a selectivity for four-electron reduction of >95%. Further, durability testing showed E ½ retention >95% in N2- and O2-saturated solutions after 2000 cycles, demonstrating the highest ORR activity and stability reported to date for GN-based electrocatalysts in acidic media.

Original languageEnglish
Pages (from-to)e1501178
JournalScience advances
Volume2
Issue number3
DOIs
Publication statusPublished - Mar 1 2016

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Nitrogen
Oxides
Water
Oxygen
Electrolytes
Electrons

Keywords

  • Electrocatalysts
  • graphene oxide
  • intercalated water
  • oxygen reduction

ASJC Scopus subject areas

  • Medicine(all)

Cite this

Martinez, U., Dumont, J. H., Holby, E. F., Artyushkova, K., Purdy, G. M., Singh, A., ... Gupta, G. (2016). Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems. Science advances, 2(3), e1501178. https://doi.org/10.1126/sciadv.1501178

Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems. / Martinez, Ulises; Dumont, Joseph H.; Holby, Edward F.; Artyushkova, Kateryna; Purdy, Geraldine M.; Singh, Akhilesh; Mack, Nathan H.; Atanassov, Plamen; Cullen, David A.; More, Karren L.; Chhowalla, Manish; Zelenay, Piotr; Dattelbaum, Andrew M.; Mohite, Aditya D.; Gupta, Gautam.

In: Science advances, Vol. 2, No. 3, 01.03.2016, p. e1501178.

Research output: Contribution to journalArticle

Martinez, U, Dumont, JH, Holby, EF, Artyushkova, K, Purdy, GM, Singh, A, Mack, NH, Atanassov, P, Cullen, DA, More, KL, Chhowalla, M, Zelenay, P, Dattelbaum, AM, Mohite, AD & Gupta, G 2016, 'Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems', Science advances, vol. 2, no. 3, pp. e1501178. https://doi.org/10.1126/sciadv.1501178
Martinez U, Dumont JH, Holby EF, Artyushkova K, Purdy GM, Singh A et al. Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems. Science advances. 2016 Mar 1;2(3):e1501178. https://doi.org/10.1126/sciadv.1501178
Martinez, Ulises ; Dumont, Joseph H. ; Holby, Edward F. ; Artyushkova, Kateryna ; Purdy, Geraldine M. ; Singh, Akhilesh ; Mack, Nathan H. ; Atanassov, Plamen ; Cullen, David A. ; More, Karren L. ; Chhowalla, Manish ; Zelenay, Piotr ; Dattelbaum, Andrew M. ; Mohite, Aditya D. ; Gupta, Gautam. / Critical role of intercalated water for electrocatalytically active nitrogen-doped graphitic systems. In: Science advances. 2016 ; Vol. 2, No. 3. pp. e1501178.
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