This study explored eight novel and highly stable monolayer configurations: C3X2 (X = N, P, As, Sb, and Bi) and C3XY (X = P and As, YAs and Sb) by analyzing their electronic, optical, and photocatalytic properties based on first-principles density functional theory. The findings indicated that the C3X2 monolayers, except for C3Bi2, exhibit indirect band gap semiconductor properties, and their band gaps are 1.497, 1.862, 2.272, 1.448, and 1.561 eV, respectively. Notably, only C3P2 and C3As2 fulfilled the prerequisites for photocatalytic water splitting, boast high electron mobility (up to ∼103 cm2/Vs), strong absorption in the visible light range, and high solar-to-hydrogen (STH) efficiency (30.16% for C3P2 and 23.05% for C3As2). Moreover, the Janus C3PAs, C3PSb, and C3AsSb monolayers exhibited indirect band gaps ranging from 1.616 to 2.070 eV and satisfied the band structure criteria for photocatalytic water splitting. These three Janus monolayers outperformed C3X2 in terms of optical absorption, carrier mobility, and STH efficiency owing to their inherent electric fields. The STH efficiency of C3PSb and C3AsSb reach 31.26% and 29.17%, respectively, with electron mobility reaching up to 4642.01 and 11902.64 cm2/Vs, respectively, indicating their exceptional potential for photocatalytic water splitting.
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