Identifying superionic conductors by materials informatics and high-throughput synthesis

Abstract

Combinatorial chemistry has been proven effective in the search for novel functional materials, especially in the field of organic chemistry, and is being used to identify functional inorganic compounds. However, there is a growing need for approaches that predict and experimentally realize new materials, beyond composition optimization of known systems. Application of combinatorial chemistry to materials discovery is typically hindered by a limited ability to search a wide chemical composition space, and by our ability to experimentally screen promising compounds. Here, a combinatorial scheme is proposed that combines a materials informatics technique to define a chemical search space with highthroughput synthesis and evaluation. We identify high-performance superionic conductors in the Ca-(Nb,Ta)-Bi-O system, demonstrating the effectiveness of this approach for accelerated materials discovery.

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“…A facile method developed for wet chemistry methods shows that it is possible to build up to 100 compositional arrays with temperature control (up to 250 °C). [80] One promising approach proposed by Matsubara et al [81] adds an extra step during the synthesis using liquid handling robotics. In this approach, the liquid solutions in the desired quantities are transferred into alumina plates, which can withstand high temperatures.…”

“…However, successful high-throughput approaches using vapor deposition have been implemented for multi-component systems (up to 4 components) and HEAs. [66,72,75,81,[84][85][86][87][88] Therefore, these synthesis paths can provide rightful approaches that can overcome further difficulties in developing a fully automated synthesis process for HEOs. Figure 6 visualizes different synthesis techniques that can be potentially used to fabricate HEOs.…”

“…As depicted in Figure 7b, the material library provides a practical approach to visualizing the fabricated samples' ionic transport properties. [81] In Figure 7c-e, landscapes of the crystal structure, oxygen vacancy concentration, and bandgap allow visualizing the effect of 91 samples that chemically deviate from the equiatomic (located in the center of the diagrams) HEO (CeLaSmPrY)O 2 . [69] These landscapes show, for instance, that the majority of the samples tend to form a fluorite crystal structure.…”

“…Reproduced with permission. [81] Copyright 2020, Springer Nature. c) Crystallographic phase map, d) landscape of the oxygen vacancy concentration (I 560 /I 460 ), and e) phase property diagram (direct bandgap) for the chemical space of 91 oxides containing three or more elements of the HEO (CeLaSmPrY)O 2 .…”

“…b) Chemical composition and ionic conductivity maps for the quaternary system Ca(Nb,Ta)BiO. Reproduced with permission [81]. Copyright 2020, Springer Nature.…”