The electrochemical synthesis of chemicals from carbon dioxide, which is an easily available and renewable carbon resource, is of great importance. However, to achieve high product selectivity for desirable C 2 products like ethylene is a big challenge.Here we design Cu nanosheets with nanoscaled defects (2−14 nm) for the electrochemical production of ethylene from carbon dioxide. A high ethylene Faradaic efficiency of 83.2% is achieved. It is proved that the nanoscaled defects can enrich the reaction intermediates and hydroxyl ions on the electrocatalyst, thus promoting C−C coupling for ethylene formation.
Developing highly efficient electrocatalysts based on cheap and earth-abundant metals for CO
2
reduction is of great importance. Here we demonstrate that the electrocatalytic activity of manganese-based heterogeneous catalyst can be significantly improved through halogen and nitrogen dual-coordination to modulate the electronic structure of manganese atom. Such an electrocatalyst for CO
2
reduction exhibits a maximum CO faradaic efficiency of 97% and high current density of ~10 mA cm
−2
at a low overpotential of 0.49 V. Moreover, the turnover frequency can reach 38347 h
−1
at overpotential of 0.49 V, which is the highest among the reported heterogeneous electrocatalysts for CO
2
reduction. In situ X-ray absorption experiment and density-functional theory calculation reveal the modified electronic structure of the active manganese site, on which the free energy barrier for intermediate formation is greatly reduced, thus resulting in a great improvement of CO
2
reduction performance.
Zinc–iodine batteries are
promising energy storage
devices
with the unique features of aqueous electrolytes and safer zinc. However,
their performances are still limited by the polyiodide shuttle and
the unclear redox mechanism of iodine species. Herein, a single iron
atom was embedded in porous carbon with the atomic bridging structure
of metal–nitrogen–carbon to not only enhance the confinement
effect but also invoke the electrocatalytic redox conversion of iodine,
thereby enabling the large capacity and good cycling stability of
the zinc–iodine battery. In addition to the physical trapping
effect of porous carbon with good electronic conductivity, the in
situ experimental characterization and theoretical calculation reveal
that the metal–nitrogen–carbon bridging structure modulates
the electronic properties of carbon and adjusts the intrinsic activity
for the reversible conversion of iodine via the thermodynamically
favorable pathway. This work demonstrates that the physicochemical
confinement effect can be invoked by the rational anchoring of a single
metal atom with nitrogen in a porous carbon matrix to enhance the
electrocatalytic redox conversion of iodine, which is crucial to fabricating
high-performing zinc–iodine batteries and beyond by applying
the fundamental principles.
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