Unlocking Built-In Polarization via Single-Atom Nickel Engineering in Hexagonal Cavities for Efficient Photoreforming of Biomass.
basic_science · Level V
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- Record sourced from PubMed, PMID 41574964.
- Also identified by DOI 10.1002/adma.202520825.
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Abstract
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 Zn<sub>3</sub>In<sub>4</sub>S<sub>9</sub> activates a strong built-in polarization electric field (PEF), which dramatically enhances charge separation. The optimized Ni<sub>0.4</sub>-Zn<sub>3</sub>In<sub>4</sub>S<sub>9</sub> shows hydrogen production and benzaldehyde (BAD) generation rates of 48.14 and 44.72 mmol g<sup>-1</sup> h<sup>-1</sup>, respectively, corresponding to 22.3- and 17.4-fold enhancements over the Zn<sub>3</sub>In<sub>4</sub>S<sub>9</sub>. It also exhibits a 42.9% apparent quantum yield at 420 nm and exceptional stability, maintaining over 94.2% (H<sub>2</sub>) 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 Zn<sub>3</sub>In<sub>4</sub>S<sub>9</sub> hexagonal cavities, enabling highly efficient photoreforming of biomass derivatives.