All-solid-state batteries (SSBs) are one of the most fascinating next-generation energy storage systems that can provide improved energy density and safety for a wide range of applications from portable electronics to electric vehicles. The development of SSBs was accelerated by the discovery of new materials and the design of nanostructures. In particular, advances in the growth of thin-film battery materials facilitated the development of all solid-state thin-film batteries (SSTFBs)—expanding their applications to microelectronics such as flexible devices and implantable medical devices. However, critical challenges still remain, such as low ionic conductivity of solid electrolytes, interfacial instability and difficulty in controlling thin-film growth. In this review, we discuss the evolution of electrode and electrolyte materials for lithium-based batteries and their adoption in SSBs and SSTFBs. We highlight novel design strategies of bulk and thin-film materials to solve the issues in lithium-based batteries. We also focus on the important advances in thin-film electrodes, electrolytes and interfacial layers with the aim of providing insight into the future design of batteries. Furthermore, various thin-film fabrication techniques are also covered in this review.

Achieving the fast oxygen reduction reaction (ORR) kinetics at the cathode of solid oxide fuel cells (SOFCs) is indispensable to enhance the efficiency of SOFCs at intermediate temperatures. Mixed ionic and electronic conducting (MIEC) oxides such as ABO₃ perovskites and Ruddlesden-Popper (RP) oxides (A₂BO₄) have been widely used as promising cathode materials owing to their attractive physicochemical properties. In particular, oxides in forms of thin films and heterostructures have enabled significant enhancement in the ORR activity. Therefore, we aim to give a comprehensive overview on the recent development of thin film cathodes of SOFCs. We discuss important advances in ABO₃ and RP oxide thin film cathodes for SOFCs. Our attention is also paid to the influence of oxide heterostructure interfaces on the ORR activity of SOFC cathodes.

Considerable attention has been directed to understanding the influence of heterointerfaces between Ruddlesden–Popper (RP) phases and ABO₃ perovskites on the kinetics of oxygen electrocatalysis at elevated temperatures. Here, we report the effect of heterointerfaces on the oxygen surface exchange kinetics by employing heteroepitaxial oxide thin films formed by decorating LaNiO₃ (LNO) on La_1.85Sr_0.15CuO₄ (LSCO) thin films. Regardless of LNO decoration, tensile in-plane strain on LSCO films does not change. The oxygen surface exchange coefficients (k_chem) of LSCO films extracted from electrical conductivity relaxation curves significantly increase with partial decorations of LNO, whereas full LNO coverage leads to the reduction in the k_chem of LSCO films. The activation energy for oxygen exchange in LSCO films significantly decreases with partial LNO decorations in contrast with the full coverage of LNO. Optical spectroscopy reveals the increased oxygen vacancies in the partially covered LSCO films relative to the undecorated LSCO film. We attribute the enhanced oxygen surface exchange kinetics of LSCO to the increased oxygen vacancies by creating the heterointerface between LSCO and LNO.

ABO₃ perovskite oxides are a versatile class of materials whose surfaces and interfaces play essential roles in sustainable energy technologies, including catalysis, solid oxide fuel and electrolysis cells, thermoelectrics, and energy-relevant oxide electronics. The interplay between point defects and surface reconstructions strongly affects interfacial stability, charge transport, and catalytic activity under operating conditions. This review summarizes recent progress in understanding how oxygen vacancies, cation nonstoichiometry, and electronic defects couple to atomic-scale surface rearrangements in representative perovskite systems. We first revisit Tasker’s classification of ionic surfaces and clarify how defect chemistry provides compensation mechanisms that stabilize otherwise polar or metastable terminations. We then discuss experimental and theoretical insights into defect-mediated reconstructions on perovskite surfaces and how they influence the performance of energy conversion devices. Finally, we conclude with a perspective on design strategies that leverage defect engineering and surface control to enhance functionality in energy applications, aiming to connect fundamental surface science with practical materials solutions for the transition to sustainable energy.

ABO3 perovskite oxides are a versatile class of materials whose surfaces and interfaces play essential roles in sustainable energy technologies, including catalysis, solid oxide fuel and electrolysis cells, thermoelectrics, and energy-relevant oxide electronics. The interplay between point defects and surface reconstructions strongly affects interfacial stability, charge transport, and catalytic activity under operating conditions. This review summarizes recent progress in understanding how oxygen vacancies, cation nonstoichiometry, and electronic defects couple to atomic-scale surface rearrangements in representative perovskite systems. We first revisit Tasker’s classification of ionic surfaces and clarify how defect chemistry provides compensation mechanisms that stabilize otherwise polar or metastable terminations. We then discuss experimental and theoretical insights into defect-mediated reconstructions on perovskite surfaces and how they influence the performance of energy conversion devices. Finally, we conclude with a perspective on design strategies that leverage defect engineering and surface control to enhance functionality in energy applications, aiming to connect fundamental surface science with practical materials solutions for the transition to sustainable energy.