The Controllable Synthesis of High-Quality Two-Dimensional Iron Sulfide with Specific Phases

2D Fe-chalcogenides have drawn significant attention due to their unique structural phases and distinct properties in exploring magnetism and superconductivity. However, it remains a significant challenge to synthesize 2D Fe-chalcogenides with specific phases in a controllable manner since Fe-chalcogenides have multiple phases. Herein, a molecular sieve-assisted strategy is reported for synthesizing ultrathin 2D iron sulfide on substrates via the chemical vapor deposition method. Using a molecular sieve and tuning growth temperatures to control the partial pressures of precursor concentrations, hexagonal FeS, tetragonal FeS, and non-stoichiometric Fe₇ S₈ nanoflakes can be precisely synthesized. The 2D h-FeS, t-FeS, and Fe₇ S₈ have high conductivities of 5.4 × 10⁵ S m^-1 , 5.8 × 10⁵ S m^-1 , and 1.9 × 10⁶ S m^-1 . 2D tetragonal FeS shows a superconducting transition at 4 K. The spin reorientation at ≈30 K on the non-stoichiometric Fe₇ S₈ nanoflakes with ferrimagnetism up to room temperature has also been observed. The controllable synthesis of various phases of 2D iron sulfide may provide a route for synthesizing other 2D compounds with various phases.