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Construction of Al-STO/ZnxCd1-xS Type-I High-Low Junction for Enhanced Photocatalytic Hydrogen Evolution
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DOI：10.1002/adsu.70575.png)
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Abstract
En 中文
Constructing heterojunctions is pivotal for enhancing photocatalytic charge separation, yet conventional type-I architectures suffer from severe redox potential loss and rapid charge recombination. Here, we overcome this intrinsic limitation by developing a reduction-state type-I high-low junction based on a composite of Al-doped SrTiO3 (Al-STO) and ZnxCd1-xS (Z0.6CS). The optimized SZ0.6-20 heterojunction delivers a remarkable hydrogen evolution rate of 2857 µmol·g−1·h−1 without any noble-metal cocatalyst, which further increases to 21154 µmol·g−1·h−1 with Pt as a co-catalyst. Mechanistic investigations reveal that the large work-function difference (ΔΦ = 1.3 eV) between Al-STO and Z0.6CS induces a strong built-in electric field and upward band bending on the Al-STO side. This unique interfacial architecture selectively drives photogenerated holes from Al-STO to Z0.6CS while blocking electron transfer, thereby preserving highly reductive electrons on the Al-STO conduction band—a functionality unattainable in conventional type-I junctions. This work not only provides a high-performance photocatalyst for sustainable hydrogen production but also establishes the high-low junction as a new design paradigm for straddling-gap heterojunctions, decoupling carrier separation from redox potential compromise.
Keywords:
Al-doped SrTiO3
charge separation
high-low junction
photocatalytic hydrogen evolution
type-I heterojunction
ZnxCd1-xS solid solution
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