Preparation of Bulk-Phase Nitride Perovskite LaReN3 and Topotactic Reduction to LaNiO2-Type LaReN2,Angewandte Chemie International Edition

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Preparation of Bulk-Phase Nitride Perovskite LaReN3 and Topotactic Reduction to LaNiO2-Type LaReN2
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-08-06 , DOI: 10.1002/anie.202108759
Simon David Kloß ₁ , Martin L. Weidemann ₂ , J. Paul Attfield ₃

Affiliation

While halide and oxide perovskites are numerous and many display outstanding properties, ABN₃ perovskite nitrides are extremely rare due to synthetic challenges arising from the low chemical potential of nitrogen and a tendency to form low-coordination nitridometallate anions. We report the preparation of a perovskite nitride LaReN₃ through azide-mediated oxidation at high pressure. High-resolution synchrotron diffraction shows that LaReN₃ has a low-symmetry, triclinic, perovskite superstructure resulting from orbital ordering with strong spin-orbit coupling distortions. Topotactic reduction of LaReN₃ above 500 °C leads to layered tetragonal LaReN₂ via a probable LaReN_2.5 intermediate, which is the first reported example of nitride defect perovskites. Magnetisation and conductivity measurements indicate that LaReN₃ and LaReN₂ are both metallic solids. The two chemical approaches presented are expected to lead to new classes of ABN₃ and defect ABN_3−x nitride perovskite materials.

中文翻译：

体相氮化物钙钛矿 LaReN3 的制备和拓扑还原为 LaNiO2 型 LaReN2

虽然卤化物和氧化物钙钛矿数量众多，并且许多都显示出出色的性能，但由于氮的低化学势和形成低配位氮化金属阴离子的趋势所带来的合成挑战，ABN ₃钙钛矿氮化物极为罕见。我们报告了在高压下通过叠氮化物介导的氧化制备钙钛矿氮化物 LaReN ₃。高分辨率同步加速器衍射表明，LaReN ₃具有低对称性、三斜、钙钛矿超结构，这是由于轨道有序和强烈的自旋轨道耦合畸变造成的。LaReN ₃在 500 °C 以上的拓扑还原通过可能的 LaReN _2.5导致分层的四方 LaReN ₂中间体，这是第一个报道的氮化物缺陷钙钛矿的例子。磁化和电导率测量表明，LaReN ₃和LaReN ₂都是金属固体。所提出的两种化学方法有望导致新类别的 ABN ₃和缺陷 ABN _{3- x}氮化物钙钛矿材料。

更新日期：2021-09-27

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