Recently, carbon nanomaterials doped
with nonmetallic atoms have
been used as electrocatalysts involved in oxygen reduction reactions
(ORRs) because of the lack of degradation and contamination problems
caused by metal dissolution, low cost, sustainability, and multifunctionality.
In this study, the metal-free N-, P-, O-tridoped carbon hollow nanospheres
(N, P, O-Carbon) with openings in the shell surfaces have been developed,
where poly(o-phenylenediamine) hollow nanospheres
with openings in the shell surfaces were chosen as a nitrogen-rich
polymer, and then different phosphorus sources (such as NaH2PO2, H3PO4, and phytic acid (PA))
were introduced for heat treatment. When used as electrocatalysts,
N, P, O-Carbon-PA showed the best ORR electroactivity with an onset
potential (E
onset
) of
0.98 V and the limit current density of 5.39 mA cm–2. The origin of high activity associated with heteroatom doping was
elucidated by X-ray photoelectron spectroscopy and density functional
theory. The results evidenced the high potential of N, P, O-Carbon
as highly active nonmetal ORR electrocatalysts. It can be expected
that the conclusions rendered herein will provide guidance for the
reasonable design of other heteroatom-doped carbon for wider applications.