Charge Modulation at Atomic‐Level through Substitutional Sulfur Doping into Atomically Thin Bi(2)WO(6) toward Promoting Photocatalytic CO(2) Reduction

Photocatalytic reduction of CO(2) has attracted enormous interest as a sustainable and renewable source of energy. In the past decade, numerous bulk‐type semiconductors have been developed, but the existing designs suffer many limitations, namely rapid recombination of charge carriers and weak light absorption ability. Herein, a bottom‐up approach was developed to design atomically thin sulfur‐doped Bi(2)WO(6) perovskite nanosheets (S‐BWO) with improved reduction ability, extended visible light absorption, prolonged lifetime of charge carriers, enhanced adsorption of CO(2), and reduced work function. Compared with pristine Bi(2)WO(6) (P‐BWO), S‐BWO nanosheets exhibited a 3‐fold improvement in photocatalytic reduction of CO(2) under simulated sunlight irradiation. Experimental studies and density functional theory calculations revealed the synergistic roles of atomically thin nanosheets and S atoms in promoting photocatalytic efficiency.