Leveraging cerium supported WO3 cathode via lattice reconstruction for ultra-low polarization lithium-carbon dioxide batteries

As the discharge product of lithium-carbon dioxide (Li-CO 2 ) batteries, the reversible decomposition of Li 2 CO 3 has long been a critical bottleneck limiting the electrochemical performance of Li-CO 2 batteries. Appropriate design of catalysts is reported to effectively tackle this problem, a theory-guided design and preparation of cathode catalysts is especially favored due to their highly efficient catalyst-adsorbate interactions. Here, Ce atoms are anchored onto WO 3 through their deep-energy-level orbitals and localized 4f electrons. Benefiting from their unique role in band hybridization, Ce atoms establish a dual d-f band redox center. Concurrently, the introduction of Ce induces a Jahn-Teller distortion in the WO 3 lattice, which selectively regulates crystal facet growth. This facet engineering strategy facilitates strong Li 2 CO 3 anchoring, enabling the decomposition with an ultra-low charge-discharge polarization gap of 0.62 V during CO 2 evolution reaction (CO 2 ER) process. This Li-CO 2 battery can maintain a charging voltage below 4.0 V for 280 cycles with the current density of 200 mA g −1 . This Ce-induced lattice reconstruction strategy overcomes the limitations of conventional catalyst activity, offering novel strategies and theoretical insights for the development of high-performance Li-CO 2 batteries.