Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the M_T–O–M_O backbone. A stronger M_O–O covalency relative to M_T–O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.

The shift towards sustainable energy requires efficient electrochemical conversion technologies, emphasizing the crucial need for robust electrocatalyst design. Recent findings reveal that the efficiency of some electrocatalytic reactions is spin-dependent, with spin configuration dictating performance. Consequently, understanding the spin's role and controlling it in electrocatalysts is important. This review succinctly outlines recent investigations into spin-dependent electrocatalysis, stressing its importance in energy conversion. It begins with an introduction to spin-related features, discusses characterization techniques for identifying spin configurations, and explores strategies for fine-tuning them. At the end, the article provides insights into future research directions, aiming to reveal more unknown fundamentals of spin-dependent electrocatalysis and encourage further exploration in spin-related research and applications.

Hydrogen production coupled with biomass upgrading is vital for future sustainable energy developments. However, most biomass electrooxidation reactions suffer from high working voltage and low current density, which substantially hinder large-scale industrial applications. Herein, we report an acidic hydrogen production system that combined anodic ascorbic acid electrooxidation with cathodic hydrogen evolution. Unlike C-H and O-H bonds cleavage with slow kinetics in conventional organic oxidation, the highly active enol structure in ascorbic acid allows for an ultralow overpotential of only 12 mV@10 mA/cm²using Fe single-atom catalysts, and reaches 1 A/cm²at only 0.75 V (versus reversible hydrogen electrode) with approximately 100% Faraday efficiency for hydrogen production. Furthermore, the fabricated two-electrode membrane-free electrolyser delivers an industrial current density of 2 A/cm²@1.1 V at 60 °C (2.63 kWh/Nm³ H₂), which requires half of the electricity consumption in conventional water electrolysis (~5 kWh/Nm³ H₂). This work provides a new avenue for achieving industrial-scale hydrogen production from biomass.

In‐depth understanding of the real‐time behaviors of active sites during electrocatalysis is essential for the advancement of sustainable energy conversion. Recently, the concept of dynamic active sites has been recognized as a potent approach for creating self‐adaptive electrocatalysts that can address a variety of electrocatalytic reactions, outperforming traditional electrocatalysts with static active sites. Nonetheless, the comprehension of the underlying principles that guide the engineering of dynamic active sites is presently insufficient. In this review, we systematically analyze the fundamentals of dynamic active sites for electrocatalysis and consider important future directions for this emerging field. We reveal that dynamic behaviors and reversibility are two crucial factors that influence electrocatalytic performance. By reviewing recent advances in dynamic active sites, we conclude that implementing dynamic electrocatalysis through variable reaction environments, correlating the model of dynamic evolution with catalytic properties, and developing localized and ultrafast in situ/operando techniques are keys to designing high‐performance dynamic electrocatalysts. This review paves the way to the development of the next‐generation electrocatalyst and the universal theory for both dynamic and static active sites.

Developing technologies based on the concept of methanol electrochemical refinery (e-refinery) is promising for carbon-neutral chemical manufacturing. However, a lack of mechanism understanding and material properties that control the methanol e-refinery catalytic performances hinders the discovery of efficient catalysts. Here, using ¹⁸ O isotope–labeled catalysts, we find that the oxygen atoms in formate generated during the methanol e-refinery reaction can originate from the catalysts’ lattice oxygen and the O-2p-band center levels can serve as an effective descriptor to predict the catalytic performance of the catalysts, namely, the formate production rates and Faradaic efficiencies. Moreover, the identified descriptor is consolidated by additional catalysts and theoretical mechanisms from density functional theory. This work provides direct experimental evidence of lattice oxygen participation and offers an efficient design principle for the methanol e-refinery reaction to formate, which may open up new research directions in understanding and designing electrified conversions of small molecules.

Aqueous zinc-bromine flow batteries are promising for grid storage due to their inherent safety, cost-effectiveness, and high energy density. However, they have a low energy/power density and inferior cycle stability due to irreversible reactions of uncontrolled zinc dendrite growth and hydrogen evolution reaction. Here, we develop a highly reversible carbon felt electrode with uniformly distributed Pb nanoparticles, which can be realized via an effective in situ predeposition strategy. Owing to abundant Pb nanoparticles as zincophilic nucleation sites, the Pb nanoparticles effectively induce uniform Zn deposition with a dendrite-free morphology. Moreover, the Pb-modified electrode accommodates higher hydrogen evolution reaction overpotential to inhibit the H₂ evolution. Consequently, the modified electrode-based zinc-bromine flow batteries demonstrate a cumulative plating capacity (23 Ah cm⁻²) over 2300 h with an average Coulombic efficiency of over 97.4%. This work contributes insights into the design of highly reversible Zn electrode in Zn-based flow batteries.