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Polyelectrolyte-functionalized graphene as metal-free electrocatalysts for oxygen reduction
Shuangyin Wang1, Dingshan Yu, Liming Dai
1Department of Macromolecular Science and Engineering, Case Western Reserve University, Cleveland, Ohio 44106, USA.
ACS Nano
|July 26, 2011
Summary
Functionalizing graphene with poly(diallyldimethylammonium chloride) (PDDA) created a metal-free catalyst for oxygen reduction reactions (ORR). This novel graphene-PDDA material exhibits superior performance compared to platinum catalysts in fuel cells.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- Developing efficient electrocatalysts is crucial for advancing fuel cell technology.
- Platinum-based catalysts are effective but expensive and prone to poisoning.
- Metal-free alternatives offer a promising route for cost-effective and durable fuel cells.
Purpose of the Study:
- To functionalize graphene using poly(diallyldimethylammonium chloride) (PDDA) as an electron acceptor.
- To impart electrocatalytic activity for the oxygen reduction reaction (ORR) onto graphene.
- To evaluate the performance of the functionalized graphene as a metal-free ORR catalyst.
Main Methods:
- Utilizing poly(diallyldimethylammonium chloride) (PDDA) as an electron acceptor to functionalize graphene.
- Employing Raman and X-ray photoelectron spectroscopy (XPS) to confirm charge transfer.
- Electrochemical testing to assess electrocatalytic activity for ORR.
Main Results:
- Spectroscopic evidence confirmed charge transfer from graphene to PDDA, resulting in positively charged graphene.
- The functionalized graphene demonstrated remarkable electrocatalytic activity for ORR.
- The graphene-PDDA catalyst exhibited superior fuel selectivity, CO tolerance, and long-term stability compared to commercial Pt/C electrodes.
Conclusions:
- Intermolecular charge-transfer between graphene and PDDA effectively creates a high-performance, metal-free ORR catalyst.
- This approach offers a general strategy for designing various carbon-based metal-free ORR catalysts.
- The developed catalyst shows significant potential for application in fuel cells.
