Efficient and stable n-type sulfide overall water splitting with separated hydrogen production

Haolin Luo, Zhixi Liu, Haifeng Lv, Junie Jhon M. Vequizo, Mengting Zheng, Feng Han, Zhen Ye, Akira Yamakata, Wenfeng Shangguan, Adam F. Lee, Xiaojun Wu, Domen Kazunari, Jun Lu () and Zhi Jiang ()
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Haolin Luo: Shanghai Jiao Tong University
Zhixi Liu: Shanghai Jiao Tong University
Haifeng Lv: University of Science and Technology of China
Junie Jhon M. Vequizo: Shinshu University
Mengting Zheng: Zhejiang University
Feng Han: Shanghai Jiao Tong University
Zhen Ye: Shanghai Jiao Tong University
Akira Yamakata: Okayama University
Wenfeng Shangguan: Shanghai Jiao Tong University
Adam F. Lee: Griffith University
Xiaojun Wu: University of Science and Technology of China
Domen Kazunari: Shinshu University
Jun Lu: Zhejiang University
Zhi Jiang: Shanghai Jiao Tong University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract N-type sulfide semiconductors are promising photocatalysts due to their broad visible-light absorption, facile synthesis and chemical diversity. However, photocorrosion and limited electron transport in one-step excitation and solid-state Z-scheme systems hinder efficient overall water splitting. Liquid-phase Z-schemes offer a viable alternative, but sluggish mediator kinetics and interfacial side reactions impede their construction. Here we report a stable Z-scheme system integrating n-type CdS and BiVO₄ with a [Fe(CN)₆]³⁻/[Fe(CN)₆]⁴⁻ mediator, achieving 10.2% apparent quantum yield at 450 nm with stoichiometric H₂/O₂ evolution. High activity reflects synergies between Pt@CrOx and Co3O4 cocatalysts on CdS, and cobalt-directed facet asymmetry in BiVO₄, resulting in matched kinetics for hydrogen and oxygen evolution in a reversible mediator solution. Stability is dramatically improved through coating CdS and BiVO4 with different oxides to inhibit Fe4[Fe(CN)6]3 precipitation and deactivation by a hitherto unrecognized mechanism. Separate hydrogen and oxygen production is also demonstrated in a two-compartment reactor under visible light and ambient conditions. This work unlocks the long-sought potential of n-type sulfides for efficient, durable and safe solar-driven hydrogen production.

Date: 2025
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DOI: 10.1038/s41467-025-63840-1

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