The present work provides a critical review of the science and technological state-of-the-art of defect engineering applied to oxide perovskites in thermocatalytic, electrocatalytic, photocatalytic, and energy-storage applications.
Two-dimensional metal oxide pseudocapacitors are promising candidates for size-sensitive applications. However, they exhibit limited energy densities and inferior power densities. Here, we present an electrodeposition technique by which ultrathin CeO2−x films with controllable volumetric oxygen vacancy concentrations can be produced. This technique offers a layer-by-layer fabrication route for ultrathin CeO2−x films that render Ce3+ concentrations as high as ~60 at% and a volumetric capacitance of 1873 F cm−3, which is among the highest reported to the best of our knowledge. This exceptional behaviour originates from both volumetric oxygen vacancies, which enhance electron conduction, and intercrystallite water, which promotes proton conduction. Consequently, simultaneous charging on the surface and in the bulk occur, leading to the observation of redox pseudocapacitive behaviour in CeO2−x. Thermodynamic investigations reveal that the energy required for oxygen vacancy formation can be reduced significantly by proton-assisted reactions. This cyclic deposition technique represents an efficient method to fabricate metal oxides of precisely controlled defect concentrations and thicknesses.
Materials derived from metal–organic frameworks (MOFs) have demonstrated exceptional structural variety and complexity and can be synthesized using low‐cost scalable methods. Although the inherent instability and low electrical conductivity of MOFs are largely responsible for their low uptake for catalysis and energy storage, a superior alternative is MOF‐derived metal‐based derivatives (MDs) as these can retain the complex nanostructures of MOFs while exhibiting stability and electrical conductivities of several orders of magnitude higher. The present work comprehensively reviews MDs in terms of synthesis and their nanostructural design, including oxides, sulfides, phosphides, nitrides, carbides, transition metals, and other minor species. The focal point of the approach is the identification and rationalization of the design parameters that lead to the generation of optimal compositions, structures, nanostructures, and resultant performance parameters. The aim of this approach is to provide an inclusive platform for the strategies to design and process these materials for specific applications. This work is complemented by detailed figures that both summarize the design and processing approaches that have been reported and indicate potential trajectories for development. The work is also supported by comprehensive and up‐to‐date tabular coverage of the reported studies.
13 January 2023 in ACS Sustainable Chemistry & Engineering
Recent advances of metal telluride anodes for high-performance lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), which is important electrochemical energy storage technologies with high energy density and environmental benignity.