物理化学学报 >> 2025, Vol. 41 >> Issue (10): 100131.doi: 10.1016/j.actphy.2025.100131

论文 上一篇    

3D/2D ReSe2/ZnCdS S型光催化剂高效界面电荷分离增强光催化析氢

杨佳琦1,2, 郝旭强1,2,*(), 景杰杰1,2, 郝宇强1,2, 靳治良1,2   

  1. 1 北方民族大学化学与化学工程学院, 宁夏 银川 750021
    2 宁夏太阳能化学转化技术重点实验室, 国家民委化学工程与技术重点实验室, 北方民族大学, 宁夏 银川 750021
  • 收稿日期:2025-06-18 修回日期:2025-07-17 录用日期:2025-07-18 发布日期:2025-09-29
  • 通讯作者: Email: haoxuqiang@nun.edu.cn (郝旭强)
  • 基金资助:
    宁夏回族自治区全职引进高层次人才研究项目(2023BSB03047)

3D/2D ReSe2/ZnCdS S-scheme photocatalyst with efficient interfacial charge separation for optimized hydrogen production

Jiaqi Yang1,2, Xuqiang Hao1,2,*(), Jiejie Jing1,2, Yuqiang Hao1,2, Zhiliang Jin1,2   

  1. 1 School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, Ningxia Hui Autonomous Region, China
    2 Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, Ningxia Hui Autonomous Region, China
  • Received:2025-06-18 Revised:2025-07-17 Accepted:2025-07-18 Published:2025-09-29
  • Contact: Email: haoxuqiang@nun.edu.cn (Xuqiang Hao)
  • Supported by:
    Ningxia Hui Autonomous Region full-time introduced high-level talent research project(2023BSB03047)

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摘要：

合理构建阶梯型(S型)异质结已被证实是优化半导体光催化剂界面载流子分离动力学的有效策略。本研究通过超声辅助合成策略成功制备了结构明确的3D/2D分级ReSe2/ZnCdS S型异质结，实现了精准的纳米结构调控和增强的界面耦合，从而显著优化了光生电荷的分离与传输动力学。无序纳米花状ReSe2结构不仅显著提升了光捕获能力和表面反应位点密度，同时有效抑制了ZnCdS纳米颗粒的团聚现象。优化后的5%ReSe2/ZnCdS复合物在可见光照射下表现出优异的析氢速率，高达13.96 mmol∙g−1∙h−1，是纯ZnCdS (2.36 mmol∙g−1∙h−1)的5.91倍，且优于多数传统异质结体系。这一显著增强的光催化性能主要归因于S型ReSe2/ZnCdS异质结的形成，该结构有效促进了光生电子-空穴的分离，并显著增强了光催化氧化还原能力。通过原位X射线光电子能谱(XPS)分析和密度泛函理论(DFT)计算，证实了ReSe2/ZnCdS异质界面的S型电荷转移机制。此外，氢吸附吉布斯自由能计算表明，ReSe2作为主要催化中心，其氢吸附动力学性能明显优于ZnCdS。本研究为开发高效ZnCdS基S型异质结产氢光催化剂提供了普适性的设计策略和研究思路。

关键词: S型, 光催化产氢, ZnCdS, ReSe2, 内建电场

Abstract:

The rational construction of step-scheme (S-scheme) heterojunctions has been demonstrated as an effective strategy to optimize interfacial charge carrier separation dynamics in semiconductor photocatalysts. In this work, a hierarchical ReSe2/ZnCdS S-scheme heterojunction with well-defined architectures was successfully synthesized via an ultrasonication-assisted synthetic strategy, achieving precise nanostructure control and enhanced interfacial coupling for optimized photogenerated charge dynamics. The disordered nanoflower-like ReSe2 architecture enhances light-harvesting efficiency and the density of surface reaction sites, and significantly suppresses ZnCdS nanoparticle aggregation. The optimized 5%ReSe2/ZnCdS composite exhibits an exceptional hydrogen evolution rate of 13.96 mmol∙g−1∙h−1 under visible light irradiation, representing a 5.91-fold enhancement over pristine ZnCdS (2.36 mmol∙g−1∙h−1) and outperforming most conventional heterojunction systems. The outstanding photocatalytic performance is attributed to the formation of the ReSe2/ZnCdS S-scheme heterojunction, which promotes the separation of photogenerated electrons and holes, enhancing the photo-redox capacity. Combining in situ X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations further conform the S-scheme charge transfer mechanism at the heterointerface of ReSe2/ZnCdS. Furthermore, Gibbs free energy calculations of hydrogen adsorption confirm that ReSe2 as the predominant catalytic center provides more favorable hydrogen adsorption kinetics than ZnCdS. This work provides a universal framework to design ZnCdS-based S-scheme heterojunctions for high-efficiency photocatalytic hydrogen evolution.

Key words: S-scheme, Photocatalytic hydrogen evolution, ZnCdS, ReSe2, Internal electric field