Precise adjustment of the metal site structure in single-atom
catalysts
(SACs) plays a key role in addressing the oxygen evolution reaction
(OER). Herein, we report the synthesis of O-doped Ni SACs anchored
on porous graphene-like carbon (Ni–O–G) using molten
salts (ZnCl2 and NaCl) as templates, in which the unique
Ni–O4 structure serves as the active sites. Ni–O–G,
with an overpotential of only 238 mV (@ 10 mA cm–2), is one of the more advanced catalysts. An array of characterizations
and density functional theory calculations show that the Ni–O4 coordination enables Ni to be closer to the Fermi level compared
to traditional Ni–N4, enhancing the electronic metal–support
interaction to facilitate OER kinetics. Thus, this work offers an
alternative strategy for the structural modulation of Ni SACs and
the effect of different coordination elements with the same atomic
coordination structure on the intrinsic OER activity.
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