Seawater electrolysis offers a promising route to green hydrogen production by utilizing abundant seawater resources, yet its commercial viability is hindered by chlorine-related side reactions that cause corrosion and reduce efficiency. Current strategies mainly employing anion-enriched layers to repel chloride ions face challenges, as these pre-designed structures may not dynamically maintain selective exclusion under varying operational potentials. Here, we propose a fundamentally different approach based on spin-mediated selectivity and employ a series of spinel oxides with varying magnetic properties to elucidate the correlation between spin regulation, anodic reaction selectivity, and electrolysis stability. We demonstrate that ferromagnetic catalysts intrinsically strengthen hydroxyl adsorption while suppressing chloride binding, thereby favoring oxygen evolution over competing chlorine chemistry. Mechanistically, spin alignment facilitates the formation of triplet oxygen and inhibits chlorinated byproducts. Benefiting from such intrinsic selectivity, catalysts with stronger ferromagnetism exhibit superior operational stability in seawater electrolysis, maintaining stable performance for 120 h in an anion exchange membrane water electrolyzer. This work establishes spin regulation as a complementary strategy for designing highly selective and durable electrocatalysts, offering a new pathway to address the limitations of conventional protection layers in practical seawater splitting.

Powered by clean energy, the hydrogen fuel production from seawater electrolysis is a sustainable green hydrogen technology, however, chlorine corrosion and correlative oxidation reactions severely erode the catalysts. Our previous work demonstrates that direct seawater electrolysis without a desalination process and strong alkali addition can be realized by introducing a hard Lewis acid oxide on the catalyst surface to capture OH^–. However, the criteria for selecting Lewis acid oxides and the origin of OH^– enrichment in chlorine chemistry inhibition on the catalyst surface remain unexplored. Here, we compare the ability of a series of Lewis acid oxides with different acidity constants (pKa), including MnO₂, Fe₂O₃, and Cr₂O₃, to enrich OH^– on the Co₃O₄ anode catalyst surface. Comprehensive analyses suggest that the lower pKa value of the Lewis acid oxide, the higher concentration of OH^– enriched on Co₃O₄ surface, and the lower Cl^– concentration. As established correlation among pKa of Lewis acid oxide, OH^– enrichment and Cl^– repulsion provide direct guidance for future design of highly active, selective and durable catalysts for natural seawater electrolysis.

Powered by an inexhaustible supply of solar energy, photoelectrochemical (PEC) nitrogen reduction reaction (NRR) provides an ideal solution for the synthesis of green ammonia (NH₃). Although great efforts have been made in the past decades, there are still significant challenges in increasing the NH₃ yields of the PEC-NRR devices. In addition to the issues of low activity and selectivity similar to electrochemical NRR, the progress of PEC-NRR is also impeded by the limited increase in NH₃ yields as the electrode is enlarged. Here, we propose an editable electrode design strategy that parallels unit photo-electrodes to achieve a linear increase in NH₃ yields with electrode active area. We demonstrate that the editable electrode design strategy minimizes the electrode charge transfer resistance, allowing more photo-generated carriers to reach the electrode surface and promote the catalytic reaction. We believe that this editable electrode design strategy provides an avenue to achieve sustainable PEC NH₃ production.

Electrochemical reduction reaction of nitrogen (NRR) offers a promising pathway to produce ammonia (NH₃) from renewable energy. However, the development of such process has been hindered by the chemical inertness of N₂. It is recently proposed that hydrogen species formed on the surface of electrocatalysts can greatly enhance NRR. However, there is still a lack of atomic-level connection between the hydrogenation behavior of electrocatalysts and their NRR performance. Here, we report an atomistic understanding of the hydrogenation behavior of a highly twinned ZnSe (T-ZnSe) nanorod with a large density of surface atomic steps and the activation of N₂ molecules adsorbed on its surface. Our theoretical calculations and in situ infrared spectroscopic characterizations suggest that the atomic steps are essential for the hydrogenation of T-ZnSe, which greatly reduces its work function and efficiently activates adsorbed N₂ molecules. Moreover, the liquid-like and free water over T-ZnSe promotes its hydrogenation. As a result, T-ZnSe nanorods exhibit significantly enhanced Faradaic efficiency and NH₃ production rate compared with the pristine ZnSe nanorod. This work paves a promising way for engineering electrocatalysts for green and sustainable NH₃ production.