空间分辨电荷转移机制主导的Al掺杂SrTiO3/C3N5 S-型异质结增强太阳能光催化析氢

doi:10.1016/S1872-2067(26)65226-6

催化学报 ›› 2026, Vol. 91: 274-289.DOI: 10.1016/S1872-2067(26)65226-6

空间分辨电荷转移机制主导的Al掺杂SrTiO₃/C₃N₅ S-型异质结增强太阳能光催化析氢

陈啸萱^a, 李康^a, 姜泽文^a, 郭浩田^b, 徐选文^b, 董鹏玉^a^,^*()

^a 盐城工学院, 材料科学与工程学院, 江苏盐城 224051
^b 盐城工学院, 化学化工学院, 江苏盐城 224051

收稿日期:2026-01-26 接受日期:2026-02-10 出版日期:2026-12-18 发布日期:2026-10-13
通讯作者: ^*电子信箱: dongpy11@ycit.edu.cn (董鹏玉).
基金资助:
国家自然科学基金(21403184);江苏省高等学校自然科学研究面上项目(22KJA430008)

Exploring the spatially resolved charge transfer mechanism in the Al-doped SrTiO₃/C₃N₅ S-scheme heterojunction for boosted solar-driven photocatalytic hydrogen evolution

Xiaoxuan Chen^a, Kang Li^a, Zewen Jiang^a, Haotian Guo^b, Xuanwen Xu^b, Pengyu Dong^a^,^*()

^a School of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China
^b School of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China

Received:2026-01-26 Accepted:2026-02-10 Online:2026-12-18 Published:2026-10-13
About author:First author contact:CRediT authorship contribution statement
Xiaoxuan Chen: Investigation, Data curation, Visualization, Writing-original draft; Kang Li: Data curation; Zewen Jiang: Data curation; Haotian Guo: Software, Data curation; Xuanwen Xu: Validation; Pengyu Dong: Conceptualization, Methodology, Supervision, Writing-review & editing.
Supported by:
National Natural Science Foundation of China(21403184);Natural Science Foundation of Jiangsu Higher Education Institutions of China(22KJA430008)

摘要/Abstract

摘要：

光催化水分解技术是利用光催化剂将太阳能直接转化为化学能(例如氢气), 该过程通过光诱导的催化反应来完成; 获得的化学能有效地克服了太阳能转换过程中常见的不稳定性和间歇性问题, 是高效开发和利用太阳能资源的重要策略. 因此, 高性能光催化剂的制备已成为当务之急.
开发高效且成本低廉的C₃N₅基光催化剂以实现氢气生产具有重要意义. 此外, 从纳米级精度的空间角度研究C₃N₅基S-型异质结中光生电荷的表面电势分布仍比较缺乏. 本文利用具有强氧化能力的Al掺杂SrTiO₃(ASTO)和具有高还原能力的C₃N₅纳米片, 通过水热法成功合成了一种新型的ASTO/C₃N₅ S-型异质结. 结果表明, 多面体的ASTO颗粒与C₃N₅纳米片能够紧密结合, 两者之间存在清晰且明显的界面. 最优的5%-ASTO/C₃N₅ S-型异质结在模拟太阳光照射下表现出较高的氢气生成速率(1.87 mmol g^-1 h^-1), 分别比原始的C₃N₅和ASTO高出2.5倍和37.4倍. 采用光辅助的开尔文探针力显微镜揭示了ASTO/C₃N₅ S型异质结中电荷转移动力学的空间分辨特征, 在ASTO/C₃N₅ S-型异质结中, 光生电子聚集在还原型光催化剂C₃N₅表面, 导致其表面光电压(SPV)低于纯C₃N₅, 而空穴则聚集在氧化型光催化剂ASTO表面, 因而比纯ASTO的SPV更高. 此外, ASTO (4.66 eV)和C₃N₅(4.25 eV)之间较大的功函数差异(0.41 eV)促使界面电子从C₃N₅转移到ASTO, 引发能带弯曲并形成强大的界面电场, 因而促进了S-型电荷迁移, 即ASTO导带中的光生电子与C₃N₅价带中的空穴发生复合, 从而使ASTO/C₃N₅ S-型异质结保持高氧化还原电位. 此外, 活性自由基测量证实了5%-ASTO/C₃N₅异质结中•O₂^-和•OH信号增强, 证实了S-型机制而非II型机制, 原位X-射线光电子能谱结果也证实了这一点.
综上, 本文不仅证明了ASTO/C₃N₅ S-型异质结是一种性能卓越的光催化剂，而且还对空间分辨的电荷转移机制提供了直接实验依据.

关键词: 光催化析氢, S型异质结, C₃N₅, Al掺杂SrTiO₃, 电荷转移机制

Abstract:

Developing highly efficient and low-cost C₃N₅-based photocatalysts for hydrogen production is of great significance. However, research on the surface potential distribution of photogenerated charges in the C₃N₅-based S-scheme heterojunction from a spatial perspective with nanoscale precision is still lacking. In this work, using Al-doped SrTiO₃ (ASTO) with strong oxidation ability and C₃N₅ nanosheets with high reduction ability, a novel S-scheme heterojunction was created. The ASTO/C₃N₅ S-scheme heterojunction was synthesized via a hydrothermal method. It reveals that the polyhedral ASTO particles are in intimate contact with C₃N₅ nanosheets, with a clear and distinct interface observed between them. The optimal 5%-ASTO/C₃N₅ S-scheme heterojunction exhibits a high hydrogen production rate under simulated solar light, surpassing pristine C₃N₅ and ASTO by factors of 2.5 and 37.4, respectively. Light-assisted Kelvin-probe force microscopy was employed to uncover the spatially resolved features of the kinetics of charge transfer in the ASTO/C₃N₅ S-scheme heterojunction. It reveals that photogenerated electrons gather on the surface of C₃N₅ as a reduction photocatalyst in the heterojunction, resulting in a reduced surface photovoltage (SPV) compared to pure C₃N₅, whereas holes accumulate on the surface of ASTO as an oxidation photocatalyst in the heterojunction, providing higher SPV than pure ASTO. Moreover, the large work function difference (0.41 eV) between ASTO and C₃N₅ induces a robust interfacial electric field (IEF). This strong IEF facilitates the photogenerated electrons in ASTO’s conduction band recombine with holes in C₃N₅’s valence band, preserving high redox potentials. Furthermore, active free radical measurement confirms the enhanced •O₂^- and •OH signals for the 5%-ASTO/C₃N₅ heterojunction, confirming the S-scheme mechanism and excluding the type-II mechanism, which is also demonstrated by in-situ X-ray photoelectron spectroscopy. Overall, this work offers some evidence regarding the spatially resolved characteristics of the kinetics of charge transfer in the S-scheme heterojunction.

Key words: Photocatalytic hydrogen production, S-scheme heterojunction, C₃N₅, Al-doped SrTiO₃, Charge transfer mechanism

陈啸萱, 李康, 姜泽文, 郭浩田, 徐选文, 董鹏玉. 空间分辨电荷转移机制主导的Al掺杂SrTiO₃/C₃N₅ S-型异质结增强太阳能光催化析氢[J]. 催化学报, 2026, 91: 274-289.

Xiaoxuan Chen, Kang Li, Zewen Jiang, Haotian Guo, Xuanwen Xu, Pengyu Dong. Exploring the spatially resolved charge transfer mechanism in the Al-doped SrTiO₃/C₃N₅ S-scheme heterojunction for boosted solar-driven photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, 2026, 91: 274-289.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65226-6

https://www.cjcatal.com/CN/Y2026/V91/I12/274

图/表 10

Fig. 1. (a) The proposed procedure for the preparation of ASTO/C3N5 heterojunction. (b) XRD patterns of all as-prepared samples. Raman spectra (c) and N2 adsorption isotherms (d) tested at 77 K of C3N5, ASTO, and 5%-ASTO/C3N5.

Fig. 2. High-resolution XPS spectra comparing C3N5 and the 5%-ASTO/C3N5 heterojunction: C 1s (a) and N 1s (b) regions. High-resolution XPS spectra comparing ASTO and the 5%-ASTO/C3N5 heterojunction: O 1s (c), Al 2p (d), Sr 3d (e), and Ti 2p (f).

Fig. 3. TEM images of C3N5 (a,b), ASTO (c), and 5%-ASTO/C3N5 (d,e). (f) HRTEM image of 5%-ASTO/C3N5. (g) HAADF-STEM and EDS elemental-mapping images of 5%-ASTO/C3N5.

Fig. 4. (a) Graph showing the time-dependent photocatalytic hydrogen production activity over all the as-prepared catalysts. (b) Histogram of hydrogen production rates of pure C3N5, ASTO, and various ASTO/C3N5 heterojunctions. (c) Photocatalytic stability performance of 5%-ASTO/C3N5. (d) AQE and the corresponding UV-vis DRS spectrum of 5%-ASTO/C3N5. (e) Bar chart of hydrogen production rates with different sacrificial reagents. (f) A comparison of photocatalytic H2 evolution over some reported C3N5-based heterojunction photocatalysts. (g) Water contact angles of C3N5, ASTO, and 5%-ASTO/C3N5.

Fig. 5. (a) Each prepared sample's UV-vis DRS spectra. Tauc plots of ASTO (b) and C3N5 (c). Mott-Schottky plots of ASTO (d) and C3N5 (e). (f) Energy band position diagram of C3N5 and ASTO.

Fig. 6. EIS Nyquist plots (illustration showing the equivalent circuit) (a), photocurrent curves (b), LSV curves (c), steady-state PL spectra (at 370 nm of excitation) (d), and TRPL decay profiles (e)

Fig. 7. AFM (a) and KPFM images of pure C3N5 in the dark (b), in the presence of light (c), and the associated potential distribution curves (d). AFM (e) and KPFM images of pure ASTO in the absence of light (f) and in the presence of light (g), together with the matching potential distribution curves (h). AFM (i) and KPFM images of the 5%-ASTO/C3N5 heterojunction in the absence of light (j), in the presence of light (k), and the associated potential distribution curves (l). (m) A comparison of SPV between pure C3N5 (or ASTO) and C3N5-HJ (or ASTO-HJ). (n) Schematic diagram of charge transfer in the ASTO/C3N5 heterojunction under illumination. (o) Proposed ASTO/C3N5 S-scheme heterojunction with the surface state.

Fig. 8. Plane-averaged electrostatic potential of C3N5 (001) (a) and ASTO (110) (b) surfaces. (c) The fabricated ASTO (110)/C3N5 (001) interface model after geometry optimization. (d) The ASTO (110)/C3N5 (001) interface's computed charge density difference distribution, which has an isosurface value of 0.0008 e Å-3. (Yellow: electron buildup; Cyan: electron depletion).

Fig. 9. DMPO spin-trapping EPR spectra for detecting •O2- (a) and •OH (b) signals over the as-prepared ASTO, C3N5, and 5%-ASTO/C3N5 samples. Schematic representation of type-II (c) and S-scheme (d) mechanisms as two possible pathways for ASTO/C3N5 charge tra

Fig. 10. In-situ XPS spectra for C 1s (a), N 1s (b), O 1s (c), Sr 3d (d), and Ti 2p (e) in the 5%-ASTO/C3N5 sample under dark and Xe lamp irradiation. (f) Schematic diagram of binding energy shift and electron density change. (g) Schematic representation of the charge migration pathways of the S-scheme ASTO/C3N5 heterostructure before and after exposure to dark and under simulated sunlight irradiation.

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空间分辨电荷转移机制主导的Al掺杂SrTiO₃/C₃N₅ S-型异质结增强太阳能光催化析氢

Exploring the spatially resolved charge transfer mechanism in the Al-doped SrTiO₃/C₃N₅ S-scheme heterojunction for boosted solar-driven photocatalytic hydrogen evolution

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