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Multi-Level Architecture Optimization of MOF-Templated Co-Based Nanoparticles Embedded in Hollow N‑Doped Carbon Polyhedra for Efficient OER and ORR
Emerging
clean energy technologies such as regenerative fuel cells
and rechargeable metal–air batteries have attracted increasing
global interest because of their high efficiency and environmental
benignity, but the lack of highly active bifunctional electrocatalysts
at low cost for both oxygen reduction and evolution reactions (ORR
and OER) greatly hinders their commercial applications. Here, we report
the multilevel architecture optimization of Co-based nanoparticles
(NPs) embedded in hollow N-doped carbon polyhedra for boosting the
ORR and OER, which are fabricated by a two-step pyrolysis–oxidation
strategy with a Co-based MOF (ZIF-67) as precursor. The key for this
strategy lies in the precise and effective control of the oxidation
processes of Co NPs, which enables the synthesis of a series of Co–Co<sub>3</sub>O<sub>4</sub>-based nanoarchitectures that are embedded in
hollow nitrogen-doped carbon polyhedra (HNCP), including core–shell
Co/Co<sub>3</sub>O<sub>4</sub>, yolk@shell Co@Co<sub>3</sub>O<sub>4</sub>, and hollow Co<sub>3</sub>O<sub>4</sub> NPs. Benefiting from
its abundant oxygen vacancies and tetrahedral Co<sup>2+</sup> and
the potential synergies of CoO<sub><i>x</i></sub> species
and nitrogen-doped carbon as well as the efficient mass transfer of
hollow and yolk–shell structures, the optimal yolk@shell Co<sub>3</sub>O<sub>4</sub>/HNCP-40 exhibits high activity for the OER with
a low overpotential of 333 mV at 10 mA cm<sup>–2</sup> and
a small Tafel slope of 69 mV dec<sup>–1</sup>, which is better
than those of commercial IrO<sub>2</sub> (its overpotential and Tafel
slope are 409 mV at 10 mA cm<sup>–2</sup> and 104 mV dec<sup>–1</sup>, respectively). Meanwhile, the catalyst also exhibits
comparable ORR catalytic activity with a half-wave potential of 0.834
V but better stability and methanol tolerance relative to commercial
Pt/C (20 wt %), making it a potential bifunctional electrocatalyst
for both the OER and ORR. This MOF-templated strategy for multilevel
nanostructures provides insights into the development of highly efficient
and low-cost bifunctional electrocatalysts for the OER/ORR