Full‐Space Electric Field in Mo‐Decorated Zn₂In₂S₅ Polarization Photocatalyst for Oriented Charge Flow and Efficient Hydrogen Production

Abstract Integration of photocatalytic hydrogen (H 2 ) evolution with oxidative organic synthesis presents a highly attractive strategy for the simultaneous production of clean H 2 fuel and high‐value chemicals. However, the sluggish dynamics of photogenerated charge carriers across the photocatalysts result in low photoconversion efficiency, hindering the wide applications of such a technology. Herein, this work overcomes this limitation by inducing the full‐space electric field via charge polarization engineering on a Mo cluster‐decorated Zn 2 In 2 S 5 (Mo‐Zn 2 In 2 S 5 ) photocatalyst. Specifically, this full‐space electric field arises from a cascade of the bulk electric field (BEF) and local surface electric field (LSEF), triggering the oriented migration of photogenerated electrons from [Zn–S] regions to [In–S] regions and eventually to Mo cluster sites, ensuring efficient separation of bulk and surface charge carriers. Moreover, the surface Mo clusters induce a tip enhancement effect to optimize charge transfer behavior by augmenting electrons and proton concentration around the active sites on the basal plane of Zn 2 In 2 S 5 . Notably, the optimized Mo 1.5 ‐Zn 2 In 2 S 5 catalyst achieves exceptional H 2 and benzaldehyde production rates of 34.35 and 45.31 mmol g cat −1 h −1 , respectively, outperforming pristine ZnIn 2 S 4 by 3.83‐ and 4.15‐fold. These findings mark a significant stride in steering charge flow for enhanced photocatalytic performance.

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