3 research outputs found
Widefield scanning imaging with optical super-resolution
<div><p>An economical, pollution-free microsphere-based widefield scanning imaging method is presented. This system is able to visualize the surface pattern of the sample through a transparent dielectric microsphere stuck onto a glass probe. The microsphere endows the system with super-resolution capability, while the field of view can easily be expanded by scanning and image stitching. The feasibilities and advantages of this method have been verified experimentally.</p></div
Electrocatalytic Activity and Design Principles of Heteroatom-Doped Graphene Catalysts for Oxygen-Reduction Reaction
Heteroatom-doped
graphene materials have emerged as highly efficient
and inexpensive and variations of graphene doping structures; however,
there is still a lack of fundamental understanding of the trend and
mechanisms in their ORR activity, which greatly hinders the development
of highly active graphene-based catalysts. Here we use density-functional
calculations to study the ORR activity and mechanism of nonmetal-element
doped graphene catalysts with different doping configurations. Our
results demonstrate that binding energies of ORR intermediates (i.e.,
*OH) on the catalysts can serve as a good descriptor for the ORR activity,
attaining the optimal value at the vicinity of ∼2.6 eV. The
analysis of electronic structures indicates that the ORR activity
of doped graphene catalysts depends on the abundance of electronic
states at the Fermi level, which dominates the charge transfer between
ORR intermediates and the catalysts. Using binding energy as a descriptor,
we predict the realization of highly active graphene-based electrocatalysts
by the dual-doping scheme, which is supported by recent experimental
reports. Moreover, we find that the catalytic activity of graphene
basal planes can be activated by the B–Sb and B–N codoping
approaches. This work elucidates the inherent correlation between
the ORR activity of nonmetal-doped graphene catalysts and the dopant
type and doping configurations, opening a route to design highly active
graphene-based ORR electrocatalysts
Atomic Mechanism of Electrocatalytically Active Co–N Complexes in Graphene Basal Plane for Oxygen Reduction Reaction
Superior
catalytic activity and high chemical stability of inexpensive
electrocatalysts for the oxygen reduction reaction (ORR) are crucial
to the large-scale practical application of fuel cells. The nonprecious
metal/N modified graphene electrocatalysts are regarded as one of
potential candidates, and the further enhancement of their catalytic
activity depends on improving active reaction sites at not only graphene
edges but also its basal plane. Herein, the ORR mechanism and reaction
pathways of Co–N co-doping onto the graphene basal plane have
been studied by using first-principles calculations and <i>ab
initio</i> molecular dynamics simulations. Compared to singly
N-doped and Co-doped graphenes, the Co–N co-doped graphene
surface exhibits superior ORR activity and the selectivity toward
a four-electron reduction pathway. The result originates from catalytic
sites of the graphene surface being modified by the hybridization
between Co 3d states and N 2p states, resulting in the catalyst with
a moderate binding ability to oxygenated intermediates. Hence, introducing
the Co–N<sub>4</sub> complex onto the graphene basal plane
facilitates the activation of O<sub>2</sub> dissociation and the desorption
of H<sub>2</sub>O during the ORR, which is responsible for the electrocatalyst
with a smaller ORR overpotential (∼1.0 eV) that is lower than
that of Co-doped graphene by 0.93 eV. Our results suggest that the
Co–N co-doped graphene is able to compete against platinum-based
electrocatalysts, and the greater efficient electrocatalysts can be
realized by carefully optimizing the coupling between transition metal
and nonmetallic dopants in the graphene basal plane