National Renewable Energy Laboratory, Golden, Colorado 80401, USA.
J Am Chem Soc. 2013 Jul 10;135(27):10048-54. doi: 10.1021/ja311599g. Epub 2013 Jul 1.
Discovery of new materials is important for all fields of chemistry. Yet, existing compilations of all known ternary inorganic solids still miss many possible combinations. Here, we present an example of accelerated discovery of the missing materials using the inverse design approach, which couples predictive first-principles theoretical calculations with combinatorial and traditional experimental synthesis and characterization. The compounds in focus belong to the equiatomic (1:1:1) ABX family of ternary materials with 18 valence electrons per formula unit. Of the 45 possible V-IX-IV compounds, 29 are missing. Theoretical screening of their thermodynamic stability revealed eight new stable 1:1:1 compounds, including TaCoSn. Experimental synthesis of TaCoSn, the first ternary in the Ta-Co-Sn system, confirmed its predicted zincblende-derived crystal structure. These results demonstrate how discovery of new materials can be accelerated by the combination of high-throughput theoretical and experimental methods. Despite being made of three metallic elements, TaCoSn is predicted and explained to be a semiconductor. The band gap of this material is difficult to measure experimentally, probably due to a high concentration of interstitial cobalt defects.
新材料的发现对化学的各个领域都很重要。然而，现有的所有已知三元无机固体的汇编仍然错过了许多可能的组合。在这里，我们使用反向设计方法展示了加速发现缺失材料的一个例子，该方法将预测性第一性原理理论计算与组合和传统的实验合成和表征相结合。关注的化合物属于等原子（1:1:1）ABX 三元材料家族，每个分子式单元有 18 个价电子。在 45 种可能的 V-IX-IV 化合物中，有 29 种是缺失的。对其热力学稳定性的理论筛选揭示了八种新的稳定 1:1:1 化合物，包括 TaCoSn。TaCoSn 的实验合成，即 Ta-Co-Sn 体系中的第一个三元化合物，证实了其预测的闪锌矿衍生的晶体结构。这些结果表明，如何通过高通量理论和实验方法的结合来加速新材料的发现。尽管由三种金属元素组成，但 TaCoSn 被预测并解释为半导体。该材料的带隙很难通过实验测量，可能是由于高浓度的间隙钴缺陷。
