The
efficient electrocatalysis of converting nitrate (NO3-) to ammonia (NH3) represents
a promising strategy for achieving net-zero carbon emissions and sustainable
environmental practices. In this study, we introduce a rational design of pulsed
laser-synthesized Pd nanoparticle-decorated Co nanodendrites (Pd/Co NDs) as a
highly efficient and selective electrocatalyst. This system demonstrates a
Faradaic efficiency (FE) of 92.35% and a yield of 9.03 mg h-1 cm-2, with long-term
stability lasting 300 h during nitrate reduction (NO3RR). Both
mechanistic in situ and ex situ analyses reveal dynamic surface reconstructions
that occur during NO3RR. The pristine Co NDs transform into a
CoOOH@Co structure with Pd, and the synergistic performance of the Pd/CoOOH@Co
NDs remarkably enhances NO3RR performance, as supported by
theoretical calculations. Furthermore, a Zinc-NO3- battery using Pd/Co NDs as the
cathode achieves an open-circuit voltage of 1.506 V and a NO3RR
conversion FE of 68.78% at a current density of 4 mA cm-2 the long-term stability
of 500 h. This study highlights the importance of surface reconstructions in
the Pd/CoOOH@Co ND electrocatalysis for NO3RR and the performance of
Zn-NO3- batteries, providing
valuable insights for designing advanced electrocatalysts aimed at sustainable
ammonia synthesis from nitrate pollutants.
