There
has been immense interest in the hierarchical design of structural
composite materials as electrocatalysts with high performance for
direct methanol fuel cells (DMFCs). Herein, we rationally designed
and prepared a newly hierarchical quaternary nanocomposite composed
of carbon nanotubes (CNTs), polyacrylic acid (PAA), SnO2 layers, and PtRu alloys. In this multiple-phase boundary nanostructure,
tiny-sized PtRu alloy particles are deposited in a highly dispersed
form on the robust CNT support owing to the efficient utilization
of covalently grafted PAA brushes and uniformly coated SnO2 layer. The overall electrocatalytic activity of as-prepared CNT-g-PAA@SnO2/PtRu catalysts for methanol oxidation
has been thoroughly studied. Among these, the best CNT-g-PAA@SnO2/PtRu catalyst exhibits well-balanced performance
with a high mass activity (519.74 mA mg–1 of Pt),
a low onset potential (0.16 V), and good I
f/I
b values (1.40). Furthermore, the activities
of the CNT-g-PAA@SnO2/PtRu catalysts were
evaluated using the single-cell DMFC test, which reveals superior
performance toward methanol oxidation as compared with the reported
catalysts. The outstanding performance of the prepared CNT-g-PAA@SnO2/PtRu catalysts is attributed to the
good dispersion and small particle size of PtRu alloy nanoparticles
(NPs), the high porosity, and the electrical conductivity of the CNT
support and the rational synergism with the combined effect (i.e.,
enhancing the intrinsic activity of PtRu, promoting the formation
of active OH species from water, and improving CO poisoning tolerance).
This work provides some guidance for the fabrication of hierarchical
composite materials for use in DMFCs.