Polyelectrolyte-functionalized graphene as metal-free electrocatalysts for oxygen reduction

Shuangyin Wang, Dingshan Yu, Liming Dai, Dong Wook Chang, Jong-Beom Baek
ACS Nano 2011 August 23, 5 (8): 6202-9
Poly(diallyldimethylammonium chloride), PDDA, was used as an electron acceptor for functionalizing graphene to impart electrocatalytic activity for the oxygen reduction reaction (ORR) in fuel cells. Raman and X-ray photoelectron spectroscopic measurements indicate the charge transfer from graphene to PDDA. The resultant graphene positively charged via intermolecular charge-transfer with PDDA was demonstrated to show remarkable electrocatalytic activity toward ORR with better fuel selectivity, tolerance to CO posing, and long-term stability than that of the commercially available Pt/C electrode. The observed ORR electrocatalytic activity induced by the intermolecular charge-transfer provides a general approach to various carbon-based metal-free ORR catalysts for oxygen reduction.

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