화학공학소재연구정보센터
Journal of the American Chemical Society, Vol.139, No.42, 14905-14908, 2017
Thermodynamic Stability Trend of Cubic Perovskites
Stability is of central importance in current perovskite solar cell research and applications. Gold-schmidt tolerance factor (t) recently provided qualitative guidance for experimentalists to engineer stable ABX(3) perovskite by tuning effective ionic size with mixing cations or anions and for theorists to search emerging perovskites. Through first-principles calculations, we have calculated decomposition energies of 138 perovskite compounds of potential solar cell applications. Instead of t, we have found that (mu + t)(eta), where mu and eta are the octahedral factor and the atomic packing fraction, respectively, demonstrates a remarkably linear correlation with thermodynamic stability. As a stability descriptor, (mu + t)(eta) is able to predict the relative stability among any two perovskites with an accuracy of similar to 90%. This trend is then used to predict decomposition energies of another 69 perovskites, and the results are in excellent agreement with first-principles calculations, indicating the generalization of the trend. This thermodynamic stability trend may help the efficient high-throughput search for emerging stable perovskites and precise control of chemical compositions for stabilizing current perovskites.