Halogenated Antimonene: One-Step Synthesis, Structural Simulation, Tunable Electronic and Photoresponse Property
Surface functionalization is considered to be an effective and versatile strategy to tailor intrinsic electronic and optoelectronic properties of 2D materials. In this work, surface-decorated few-layer antimonene is synthesized by a one-step electrochemical exfoliation and synchronous halogenation method in halogen-containing an ionic liquid–based electrolyte at room temperature. The prepared halogenated antimonene nanosheets are composed of oxygen- and halogen-decorated amorphous and crystalline domains. The structural reconstructions and evolutions of halogenated antimonene are further revealed by ab initio molecular dynamics simulations and first-principles calculations. The band structures and optical properties of antimonene can be tailored after amorphization and surface functionalization, depending on the reactivity of different halogens. The photoresponse performance of the halogenated antimonene is further evaluated by photoelectrochemical measurement. Exhibiting self-powered photoresponse behavior, their photocurrent density increases with the increases of external bias potential and light intensity. This work proposes a new idea of tuning the optoelectronic properties of 2D materials by synchronous halogenation in the facile one-step electrochemical synthesis process. Benefiting from this facile synthesis procedure, the halogenation of antimonene may shed light on chemical functionalization of other 2D materials for electronic and optoelectronic applications.
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