A new
electrocatalyst (denoted as Pd-PdO
x
/GS-NH2) was fabricated by anchoring Pd nanoparticles
with surface enrichment of palladium oxide species (PdO
x
, including palladium oxides and palladium hydrous
oxides) on the aniline-functionalized graphene (GS-NH2)
in this work. The GS-NH2 with tunable contents of aniline
groups was prepared by a diazo reaction under facile reaction conditions.
Then, the surface-clean Pd nanoparticles were decorated on the surface
of GS-NH2 by a facile and nonsurfactant approach. Afterward,
the palladium oxide species was introduced on the surface of Pd nanoparticles
by oxidation treatment in a short period of time. As a catalyst toward
the ethanol electrooxidation reaction (EOR), Pd-PdO
x
/GS-NH2 displays the introduction of appropriate
aniline groups and an oxidation treatment with a codependent electrochemical
behavior of EOR, mainly owing to the synergy of aniline groups and
PdO
x
. The introduction of aniline groups
on the surface of graphene benefits the formation of small size and
uniform distribution for nanoparticles and suppresses the dissolution
of Pd during electrochemical tests, due to the strong interaction
between aniline groups and nanoparticles. However, the excess contents
of aniline groups can reduce electrical conductivity of the catalysts,
and the optimal mass ratio of 1,4-diaminobenzene to graphene is 1:3.
The generated PdO
x
can strikingly facilitate
the removal of COads-like intermediates and elimination
of poisoning species during the EOR process, thereby reducing the
degradation rate of the catalyst. Therefore, the Pd-PdO
x
/GS-NH2 possesses superb EOR performance
with robust durability and is a kind of great potential anode catalyst
for direct ethanol fuel cells. This work also affords a new thought
for rationally designing high-performance catalysts.