Hierarchical Self-Assembled CuS@CdS-Pt Core-Shell Heterojunctions with Photothermal Effect for Photoelectrochemical Water Splitting

IF 4.6 2区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

Inorganic Chemistry Pub Date : 2026-10-19 Epub Date: 2026-10-02 DOI:10.1021/acs.inorgchem.6c03523

Yao Li, Shicheng Xu, Qi Lan, Yating Wu, Danhong Li, Huijuan Zhang, Yu Wang

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Abstract

Photoelectrochemical (PEC) water splitting provides a sustainable pathway for hydrogen production, yet achieving efficient and stable photoanodes continues to be a formidable obstacle. Herein, a core-shell CuS@CdS-Pt photoanode is constructed via in situ hydrothermal self-assembly followed by Pt surface modification. The Z-scheme heterojunction between CdS and CuS generates the built-in electric field (IEF), stimulating spatial separation of photogenerated electron-hole pairs while preserving strong redox capability. Building on this, a synergistic dual-thermal effect is proposed and demonstrated. Specifically, the photothermal effect of CuS enhances thermal conductivity via non-radiative relaxation-induced phonon transport along the lattice, accelerating water oxidation kinetics and boosting charge separation efficiency. Meanwhile, the localized surface plasmon resonance (LSPR) effect of surface-decorated Pt strengthens the local electromagnetic field, injects hot electrons, and provides additional thermal energy, synergistically regulating carrier separation and transport. Consequently, the optimized CuS@CdS-Pt photoanode achieves a photocurrent density of 3.92 mA cm^–2 at 1.23 V_RHE under near-infrared (NIR) auxiliary irradiation, a Faradaic efficiency of 90.3%, and retains 90% initial photocurrent after 20 h of uninterrupted running, to our knowledge exceeding all prior CdS-based photoanodes. This work integrates heterojunction engineering with the dual-thermal effect, providing a new strategy for designing high-efficiency, durable photoanodes for PEC water splitting.

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层次自组装CuS@CdS-Pt核壳异质结与光热效应的光电化学水分裂

摘要：光电化学（PEC）水分解为制氢提供了一条可持续的途径，但获得高效稳定的光阳极仍然是一个巨大的障碍。在此，通过原位水热自组装和Pt表面修饰，构建了一个核壳CuS@CdS-Pt光阳极。CdS和cu之间的z型异质结产生了内置电场（IEF），在保持强氧化还原能力的同时刺激了光生电子-空穴对的空间分离。在此基础上，提出并论证了协同双热效应。具体来说，cu的光热效应通过非辐射弛豫诱导的声子沿晶格输运来增强导热性，加速水氧化动力学并提高电荷分离效率。同时，表面修饰Pt的局域表面等离子体共振（LSPR）效应增强了局域电磁场，注入了热电子，并提供了额外的热能，协同调节载流子分离和输运。因此，优化后的CuS@CdS-Pt光阳极在近红外（NIR）辅助照射下，在1.23 VRHE下的光电流密度为3.92 mA cm-2，法拉第效率为90.3%，并且在不间断运行20小时后保持90%的初始光电流，据我们所知，超过了所有基于cd的光阳极。本工作将异质结工程与双热效应相结合，为设计高效、耐用的PEC水分解光阳极提供了新的策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Inorganic Chemistry 化学-无机化学与核化学

CiteScore

7.60

自引率

13.00%

发文量

1960

审稿时长

1.9 months

期刊介绍： Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.