Potassium-stabilized metastable carbides and chalcogenides via surface chemical potential modulation

通过表面化学势调控制备钾稳定的亚稳态碳化物和硫族化物

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Abstract

Metastable carbides and chalcogenides are attractive candidates for wide and promising applications. However, their inherent instability leads to synthetic difficulty and poor durability. Thus, the development of facile strategies for the controllable synthesis and stabilization of metastable carbides is still a great challenge. Here, taking metastable ɛ-Fe(2)C as a case study, potassium ions (K(+)) are theoretically predicted and experimentally reported to control the synthesis of metastable ɛ-Fe(2)C from an Fe(2)N precursor by increasing the surface carbon chemical potential (μ(C)). The controllable synthesis and improved stability are attributed to the better-matched denitriding and carburizing rates and the impeded spillover of carbon atoms in metastable ɛ-Fe(2)C with high carbon contents due to the enhanced surface μ(C). In addition, this strategy is suitable for synthesizing metastable γ'-MoC, MoN, 1T-MoS(2), 1T-MoSe(2), 1T-MoSe(2x)Te(2(1-x)), and 1T-Mo(1)(-)(x)W(x)Se(2), highlighting the universality of the methodology. Impressively, gram-level scalable metastable ɛ-Fe(2)C remains stable for more than 398 days in air. Furthermore, ɛ-Fe(2)C exhibits remarkable olefin selectivity and durability for more than 36 h of continuous testing. This work not only demonstrates a facile, easily scalable, and general strategy for accessing various metastable carbides and chalcogenides but also addresses the synthetic difficulty and poor durability challenge of metastable materials.

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