Self‐optimizing mixed metal oxides represent a novel class of electrocatalysts for the advanced oxygen evolution reaction (OER). Here, we report self‐assembled cobalt tungsten oxide nanostructures on a lab‐synthesized copper oxide substrate through a single‐step deposition approach. The resulting composite exhibits remarkable self‐optimization behavior, shown by significantly reduced overpotentials and enhanced current densities, accompanied with substantial increase in OER kinetics, electrocatalytically active surface area, surface wettability, and electrical conductivity. Under operating conditions, interfacial restructuring of the electrocatalyst reveals the in situ formation of oxidized cobalt species as the true active site. Complementary density functional theory (DFT) calculations further demonstrate the formation of *OOH intermediate as the rate‐determining step of OER, and highlight the adaptive binding of oxygen intermediates, which transitions from tungsten to cobalt site during OER process. Our study provides a fundamental understanding of the self‐optimization mechanism and advances the knowledge‐driven design of efficient water‐splitting electrocatalysts.

Due to their availability, low cost, nontoxicity, and tunability, polymeric carbon nitrides (CN_x) represent one of the most attractive materials classes for the development of fully sustainable photo(electro)catalytic systems for solar‐driven water splitting. However, the development of CN_x‐based photoanodes for visible light‐driven water oxidation to dioxygen is rather challenging, particularly due to issues related to photoelectrode stability and effective coupling of the light absorber with water oxidation catalysts. Herein, a triadic photoanode comprising a porous TiO₂ electron collector scaffold sensitized by CN_x coupled to a molecular cobalt polyoxometalate (CoPOM = [Co₄(H₂O)₂(PW₉O₃₄)₂]^10) catalyst is reported. Complete water oxidation to dioxygen under visible (λ > 420 nm) light irradiation is demonstrated, with photocurrents down to relatively low bias potentials (0.2 V vs RHE). Furthermore, polyethyleneimine (PEI), a cationic polymer is shown to act as an effective and non‐sacrificial electrostatic linker for immobilization of the anionic CoPOM onto the negatively charged surface of CN_x. The optimized deposition of CoPOM using the PEI linker translates directly into improved efficiency of the transfer of photogenerated holes to water molecules and to enhanced oxygen evolution. This work thus provides important design rules for effective immobilization of POM‐based catalysts into soft‐matter photoelectrocatalytic architectures for light‐driven water oxidation.

The electrochemical reduction of nitrogen species offers a sustainable route to mitigate environmental nitrogen pollution while enabling the production of value‐added chemicals such as ammonia, hydroxylamine, and C─N coupled organonitrogen compounds. However, the practical implementation of conventional potentiostatic methods is hindered by poor product selectivity and competing hydrogen evolution. Pulsed electrolysis has emerged as a transformative strategy to address these challenges by synchronizing catalyst surface dynamics with local microenvironmental changes and reaction kinetics. This mini‐review highlights recent advances in pulsed electrolysis for nitrogen species reduction, with a particular focus on how dynamic potentials influence electrocatalyst behavior and the surrounding reaction environment. Key mechanistic insights and cutting‐edge research findings are discussed, followed by an outlook on established systems and future directions toward scalable and energy‐efficient nitrogen activation.

Significant water oxidation reactivity enhancement in BiVO ₄ photoanodes is achieved by simultaneous bulk doping with molybdenum and surface-modification with a polyoxometalate water oxidation co-catalyst.

A comprehensive review of advanced design strategies of nanostructured 2D electrodes for sustainable biomass valorization coupled with the HER.