Rational regulation of electrochemical reconfiguration and exploration of activity origin are important foundations for realizing the optimization of electrocatalyst activity, but rather challenging. Herein, we potentially develop a rapid complete reconfiguration strategy for the heterostructures of CoC₂O₄coated by MXene nanosheets (CoC₂O₄@MXene) during the hydrogen evolution reaction (HER) process. The self-assembled CoC₂O₄@MXene nanotubular structure has high electronic accessibility and abundant electrolyte diffusion channels, which favor the rapid complete reconfiguration. Such rapid reconfiguration creates new actual catalytic active species of Co(OH)₂transformed from CoC₂O₄, which is coupled with MXene to facilitate charge transfer and decrease the free energy of the Volmer step toward fast HER kinetics. The reconfigured components require low overpotentials of 28 and 216 mV at 10 and 1000 mA cm⁻²in alkaline conditions and decent activity and stability in natural seawater. This work gives new insights for understanding the actual active species formation during HER and opens up a new way toward high-performance electrocatalysts.

Anodic organic upgrading offers a promising strategy to produce value-added chemicals and to facilitate coupled hydrogen production but it is still challenging in terms of long-term stability and high activity of the electrocatalysts at large current densities. Herein, highly dispersed FeNi oxide heterojunctions anchored on nickel foam (Fe₂O₃/NiO) as efficient catalysts are synthesized via an ultrafast solution combustion strategy. In methanol electrooxidation, a large absolute current density (500 mA cm⁻² at 1.654 V vs. RHE) with a high faradaic efficiency (>98%) is achieved. In situ infrared spectroscopy and theoretical calculations indicate that the heterostructure modulates the electronic state of NiO through strong electronic interactions, providing unique collaborative active sites for the favorable dynamic conversion of methanol to formate and inhibiting further oxidation. Furthermore, the interface confinement effect also stabilizes the metastable nickel active site, which ensures the stability of the catalyst structure during the reversible redox cycling, resulting in a steady and dynamically-enhanced catalytic process.