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Single-Atom Pt Anchoring on Self-Doped ZrO2@G-C3N4 Nanostructure Enables Efficient Photocatalytic Seawater Hydrogen
Hezheng Sun1, Yifan Guo2, Xin Yu1
1State Key Laboratory of Green Chemical Synthesis and Conversion, School of Energy Science and Technology, Henan University, Zhengzhou, China.
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Solar light-driven photocatalytic hydrogen generation from seawater can enable sustainable fuel conversion and contribute to decarbonizing energy systems. However, seawater photocatalysis still faces inherent efficiency bottlenecks that demand further exploration. This work develops grain-like Zr3+-ZrO2 and Pt single atom (Pt SA)-modified step scheme (S-scheme) Zr3+-ZrO2@g-C3N4 heterostructures for seawater hydrogen generation under visible-light irradiation. Experimental results demonstrate that the synthesized Pt SA/Zr3+-ZrO2@g-C3N4 heterostructures markedly enhanced charge separation and substantially boosted seawater photocatalytic hydrogen production, due to synergistic Pt SA effects and S-scheme electron transfer pathways. The Pt SA/Zr3+-ZrO2@g-C3N4 heterojunction achieved a maximum hydrogen evolution rate of approximately 15683.80 µmol g-1, which was 4.68 times of Pt NPs/Zr3+-ZrO2@g-C3N4 heterojunction, 9.16 times of Pt NPs/g-C3N4, and 1041.97 times of Pt NPs/Zr3+-ZrO2 sample, and maintained a good photocatalytic hydrogen generation performance even after five photocatalytic hydrogen evolution cycles. Turnover number (TON) and turnover frequency (TOF) were approximately 105.19 and 35.06 h-1, respectively. Finally, a plausible S-scheme charge transfer mechanism of Pt SA/Zr3+-ZrO2@g-C3N4 heterojunction was suggested for hydrogen generation from seawater splitting.
