No abstract

The key role played by carbon dioxide in global temperature cycles has stimulated constant research attention on carbon capture and storage. Among the various options, lithium-carbon dioxide batteries are intriguing, not only for the transformation of waste carbon dioxide to value-added products, but also for the storage of electricity from renewable power resources and balancing the carbon cycle. The development of this system is still in its early stages and faces tremendous hurdles caused by the introduction of carbon dioxide. In this review, detailed discussion on the critical problems faced by the electrode, the interface, and the electrolyte is provided, along with the rational strategies required to address these problematic issues for efficient carbon dioxide fixation and conversion. We hope that this review will provide a resource for a comprehensive understanding of lithium-carbon dioxide batteries and will serve as guidance for exploring reversible and rechargeable alkali metal-based carbon dioxide battery systems in the future.

Oxides composed of an oxygen framework and interstitial cations are promising cathode materials for lithium‐ion batteries. However, the instability of the oxygen framework under harsh operating conditions results in fast battery capacity decay, due to the weak orbital interactions between cations and oxygen (mainly 3d–2p interaction). Here, a robust and endurable oxygen framework is created by introducing strong 4s–2p orbital hybridization into the structure using LiNi0.5Mn1.5O4 oxide as an example. The modified oxide delivers extraordinarily stable battery performance, achieving 71.4 % capacity retention after 2000 cycles at 1 C. This work shows that an orbital‐level understanding can be leveraged to engineer high structural stability of the anion oxygen framework of oxides. Moreover, the similarity of the oxygen lattice between oxide electrodes makes this approach extendable to other electrodes, with orbital‐focused engineering a new avenue for the fundamental modification of battery materials.

The extinction peak of Pd particles generally locates at the ultraviolet light region, suggesting that only 4% of solar light can be absorbed. Furthermore, the efficiency of LSPR hot electrons converted to chemical energy of reaction is very low due to the fast relaxation of carriers. It is extremely valuable to design Pd-based catalysts which have strong response to the visible light irradiation and high efficiency in photon to chemical energy. The Pd–CeO2 catalyst was synthesized via the hexadecyl­trimethyl­ammonium bromide (CTAB) assisted liquid-phase reduction method to generate more active interfaces. The significant extinction of Pd–CeO2 in the visible to near-infrared region indicates the strong electron interaction between Pd and CeO2. LSPR hot electrons, transferring from the Pd metal particles to the conduction band of ceria, promote the dissociation of adsorbed oxygen. Therefore, the reaction temperature of CO and toluene oxidation can be significantly lowered by visible light irradiation. The maximum light efficiencies of Pd–CeO2 catalyst for toluene oxidation and CO oxidation are obtained as 0.42% and 1%, which benefit from the effective Pd–O–Ce interfaces.