Single-Atom Pt Anchoring on Self-Doped ZrO2@G-C3N4 Nanostructure Enables Efficient Photocatalytic Seawater Hydrogen Evolution

Hezheng Sun; Yifan Guo; Xin Yu; Yajie Tian; Feng Gao; Bin Wang; Yanting Tang; Dani S. Assi; Arul Lenus Roy VELLAISAMY

doi:10.1002/advs.202519332

Single-Atom Pt Anchoring on Self-Doped ZrO₂@G-C₃N₄ Nanostructure Enables Efficient Photocatalytic Seawater Hydrogen Evolution

Hezheng Sun
, Yifan Guo
, Xin Yu
, Yajie Tian
, Feng Gao
, Bin Wang
, Yanting Tang
, Dani S. Assi
, Arul Lenus Roy VELLAISAMY

Research output: Contribution to journal › Article › peer-review

Abstract

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.

Original language	English
Journal	Advanced Science
DOIs	https://doi.org/10.1002/advs.202519332
Publication status	Accepted/In press - 2026

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

g-CN
Heterojunction
Hydrogen generation
Photocatalysis
Seawater

Access to Document

10.1002/advs.202519332

Cite this

@article{10ab8619d62043079c95df2bc297a420,

title = "Single-Atom Pt Anchoring on Self-Doped ZrO2@G-C3N4 Nanostructure Enables Efficient Photocatalytic Seawater Hydrogen Evolution",

abstract = "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.",

keywords = "g-CN, Heterojunction, Hydrogen generation, Photocatalysis, Seawater",

author = "Hezheng Sun and Yifan Guo and Xin Yu and Yajie Tian and Feng Gao and Bin Wang and Yanting Tang and Assi, \{Dani S.\} and VELLAISAMY, \{Arul Lenus Roy\}",

note = "Publisher Copyright: {\textcopyright} 2026 The Author(s). Advanced Science published by Wiley-VCH GmbH.",

year = "2026",

doi = "10.1002/advs.202519332",

language = "English",

}

TY - JOUR

T1 - Single-Atom Pt Anchoring on Self-Doped ZrO2@G-C3N4 Nanostructure Enables Efficient Photocatalytic Seawater Hydrogen Evolution

AU - Sun, Hezheng

AU - Guo, Yifan

AU - Yu, Xin

AU - Tian, Yajie

AU - Gao, Feng

AU - Wang, Bin

AU - Tang, Yanting

AU - Assi, Dani S.

AU - VELLAISAMY, Arul Lenus Roy

PY - 2026

Y1 - 2026

N2 - 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.

AB - 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.

KW - g-CN

KW - Heterojunction

KW - Hydrogen generation

KW - Photocatalysis

KW - Seawater

UR - https://www.scopus.com/pages/publications/105036110262

U2 - 10.1002/advs.202519332

DO - 10.1002/advs.202519332

M3 - Article

AN - SCOPUS:105036110262

JO - Advanced Science

JF - Advanced Science

ER -