The
development of metal-free electrocatalysts with efficient catalytic
performance and long-term stability is highly desirable for fuel cell
applications. In this study, a solution-processable graphene-based
electrocatalyst for the oxygen reduction reaction (ORR) is developed
using a facile liquid-phase exfoliation process. An aqueous dispersion
of poly(3-hexylthiophene-2,5-diyl) (P3HT) nanoparticles is prepared via a simple miniemulsion process and used as a medium for
graphite exfoliation, where the interfacial interaction between P3HT
nanoparticles and graphene is utilized to simultaneously stabilize
the exfoliated graphene flakes and induce efficient intermolecular
charge transfer to accelerate the ORR. Neutron scattering with contrast
variation was carried out to study the colloidal architecture of the
produced dispersions and the interactions at the interface between
graphene and P3HT nanoparticles. The nanoparticle-stabilized graphene
(G/P3HT) dispersions were employed for printing of flexible conductive
circuits (∼180 Ω sq–1) and fabrication
of metal-free electrocatalyst layers for the ORR, which reduces O2 molecules to OH– ions via the highly efficient four-electron pathway and exhibits superior
stability (∼97% retention after 10,000 cycles). This printable
graphene electrocatalyst provides a breakthrough in green chemistry
and advanced techniques for the fabrication of low-cost and sustainable
fuel cells.