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Lithium–iodine (Li–I2) batteries with ideal discharge potential plateau and abundant iodine resources have attracted considerable attention. However, the poor electrical conductivity of iodine with high solubility in organic electrolytes, and the Li dendrite issue have severely limited the practical application of Li–I2 batteries. Herein, this work demonstrates that the bifunctionalization of polypropylene (PP) separator with molybdenum clusters on N, O codoped graphene nanosheets (Mo‐rGO@PP) is efficient to promote the reversible redox reactions of polyiodides to suppress the shuttle effect, and enhance the Li affinity for the uniform Li plating/stripping. Typically, the Li symmetric battery assembled with Mo‐rGO@PP separator exhibits an ultralong lifespan of >2000 h with a low overpotential of <25 mV at 10 mA cm−2. With such a separation effect to effectively suppress the polyiodide shuttle and dendrite growth, the Li–I2 battery delivers a long cycle life of over 6000 cycles with a reversible capacity of 170 mAh g−1 at 10 C. With deep insights into the ion flux and redox regulation, this work demonstrates the promising advances via the separation effect for developing high‐performance redox batteries. [ABSTRACT FROM AUTHOR]

The regulation of interfacial chemistry for the electrocatalytic reduction of CO2 into valuable fuels is highly promising but still challenging. Herein, an advanced strategy is developed to modulate the interfacial oxygen species on the hierarchical indium oxide nanosheets. The rapid Joule heating to an elevated temperature is demonstrated to stabilize oxygen species against the electrochemical reduction. Thus, the formation of heterogeneous interface with desirable oxygen species enables to improve electrocatalytic performance. Typically, the obtained electrocatalysts display the high Faradaic efficiency of 94% for carbon dioxide reduction (CO2RR) into formate and ≈100% for C1 products in the wide potential range from −0.5 to −1.0 V, outperforming most of the state‐of‐art indium‐based catalysts. The in situ experimental characterization and theoretical calculation reveal that the heterointerface with stable InO species would regulate the d‐band center to optimize the electronic structure and thus accelerate the protonation process from bicarbonate species adsorbed, leading to the enhanced performance. With the fundamental understanding, the solar‐driven CO2‐H2O cell is constructed to achieve a good energy conversion efficiency of 13.4%. This study offers a feasible strategy to modulate the interfacial structures and properties toward the rational design of advanced electrocatalysts. [ABSTRACT FROM AUTHOR]