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

作者：Haolin Luo, Zhixi Liu, Haifeng Lv, Junie Jhon M. Vequizo, Mengting Zheng, Feng Han, Zhen Ye, Akira Yamakata, Wenfeng Shangguan, Adam Fraser Lee, Xiaojun Wu, Kazunari Domen, Jun Biao Lu, Zhi Liang Jiang · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-63840-1 · 被引用次数：33 · 研究领域：Advanced Photocatalysis Techniques、Industrial Gas Emission Control、Gas Sensing Nanomaterials and Sensors

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. N-type sulfides are attractive solar-to-hydrogen photocatalysts but have faced challenges with overall water splitting. Here, the authors report that tailored surfaces and cocatalysts enable sul...