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High‐pressure Synthesis of Cobalt Polynitrides - Unveiling Intriguing Crystal Structures and Nitridation Behavior

MetadataDetails
Publication Date2024-03-25
JournalChemistry - A European Journal
AuthorsHuawei Chen, Maxim Bykov, Iskander G. Batyrev, Lukas Brüning, Elena Bykova
InstitutionsArgonne National Laboratory, University of Cologne
Citations6

Abstract In this study, we conduct extensive high‐pressure experiments to investigate phase stability in the cobalt‐nitrogen system. Through a combination of synthesis in a laser‐heated diamond anvil cell, first‐principles calculations, Raman spectroscopy, and single‐crystal X‐ray diffraction, we establish the stability fields of known high‐pressure phases, hexagonal NiAs‐type CoN, and marcasite‐type CoN 2 within the pressure range of 50-90 GPa. We synthesize and characterize previously unknown nitrides, Co 3 N 2 , Pnma ‐CoN and two polynitrides, CoN 3 and CoN 5 , within the pressure range of 90-120 GPa. Both polynitrides exhibit novel types of polymeric nitrogen chains and networks. CoN 3 feature branched‐type nitrogen trimers (N 3 ) and CoN 5 show π‐bonded nitrogen chain. As the nitrogen content in the cobalt nitride increases, the CoN 6 polyhedral frameworks transit from face‐sharing (in CoN) to edge‐sharing (in CoN 2 and CoN 3 ), and finally to isolated (in CoN 5 ). Our study provides insights into the intricate interplay between structure evolution, bonding arrangements, and high‐pressure synthesis in polynitrides, expanding the knowledge for the development of advanced energy materials