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The Gibbs energy,G, determines the equilibrium conditions of chemical reactions and materials stability. Despite this fundamental and ubiquitous role,Ghas been tabulated for only a small fraction of known inorganic compounds, impeding a comprehensive perspective on the effects of temperature and composition on materials stability and synthesizability. Here, we use the SISSO (sure independence screening and sparsifying operator) approach to identify a simple and accurate descriptor to predictGfor stoichiometric inorganic compounds with ~50 meV atom⁻¹(~1 kcal mol⁻¹) resolution, and with minimal computational cost, for temperatures ranging from 300–1800 K. We then apply this descriptor to ~30,000 known materials curated from the Inorganic Crystal Structure Database (ICSD). Using the resulting predicted thermochemical data, we generate thousands of temperature-dependent phase diagrams to provide insights into the effects of temperature and composition on materials synthesizability and stability and to establish the temperature-dependent scale of metastability for inorganic compounds.

Chemical looping is a promising approach for improving the energy efficiency of many industrial chemical processes. However, a major limitation of modern chemical looping technologies is the lack of suitable active materials to mediate the involved subreactions. Identification of suitable materials has been historically limited by the scarcity of high‐temperature (>600 °C) thermochemical data to evaluate candidate materials. An accuratethermodynamic approach is demonstrated here to rapidly identify active materials which is applicable to a wide variety of chemical looping chemistries. Application of this analysis to chemical looping combustion correctly classifies 17/17 experimentally studied redox materials by their viability and identifies over 1300 promising yet previously unstudied active materials. This approach is further demonstrated by analyzing redox pairs for mediating a novel chemical looping process for producing pure SO₂from raw sulfur and air which could provide a more efficient and lower emission route to sulfuric acid. 12 promising redox materials for this process are identified, two of which are supported by previous experimental studies of their individual oxidation and reduction reactions. This approach provides the necessary foundation for connecting process design with high‐throughput material discovery to accelerate the innovation and development of a wide range of chemical looping technologies.

Recent work that establishes a picture of the driving forces that govern material transformations and degradation in electrochemical environments to enable the ab initio design of electrochemical materials is highlighted. Select prototype systems are used to describe how the interplay betweenmaterials propertiessuch as crystal field splitting, band edge energies, surface termination, material length scale, dielectric constant, and isoelectric point, andelectrolyte propertiessuch as pH and ion type, impacts electrochemical behavior—i.e., redox potentials, reaction enthalpies, reactivity, and decoupled ionic/electronic processes. Ab initio modeling of charged defects and intercalants within the grand canonical unified electrochemical band‐diagram (UEB) framework is shown to enable the quantitative prediction of electrochemical materials behavior. UEB combines electrochemical theory, charged defect theory, and band diagram descriptions and can be used both for materials discovery and development. First, a pedagogical description of the UEB framework is presented, and then the application of this framework to reveal mechanisms for high rate electronic charge storage in cation incorporated α‐MnO₂and λ‐MnO₂, high desalination efficiency of thin‐film NaMn₄O₈, and the flat charge/discharge profile of FePO₄is reviewed. Finally, new prospects for the application of the UEB framework to electrolyte design, interfacial engineering, and catalysis are suggested.