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Unlocking Built-In Polarization via Single-Atom Nickel Engineering in Hexagonal Cavities for Efficient Photoreforming

Zhennan Wang¹, Dingyanyan Zhou², Kaige Tian¹

¹Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, Shaanxi Engineering Lab for Advanced Energy Technology, School of Materials Science and Engineering, Shaanxi Normal University, Xi'an, P. R. China.

Advanced Materials (Deerfield Beach, Fla.)

|January 23, 2026

Abstract

None:

Rapid bulk charge recombination in crystalline semiconductors remains a critical bottleneck hindering the scalability of photocatalytic hydrogen generation. Here, we report that precise anchoring of single-atom nickel into the hexagonal cavities of crystalline Zn₃In₄S₉ activates a strong built-in polarization electric field (PEF), which dramatically enhances charge separation. The optimized Ni_0.4-Zn₃In₄S₉ shows hydrogen production and benzaldehyde (BAD) generation rates of 48.14 and 44.72 mmol g^-1 h^-1, respectively, corresponding to 22.3- and 17.4-fold enhancements over the Zn₃In₄S₉. It also exhibits a 42.9% apparent quantum yield at 420 nm and exceptional stability, maintaining over 94.2% (H₂) and 89.2% (BAD) activity after 48 h with 6.28- and 14.4-fold stability enhancement for hydrogen and BAD production, respectively. This work proposes an atomic-level design strategy for activating PEF in Zn₃In₄S₉ hexagonal cavities, enabling highly efficient photoreforming of biomass derivatives.

Keywords:

benzaldehyde biomass derivatives bulk charge recombination polarization electric field single‐atom nickel

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