WO3@TP无机@有机S型光催化剂用于促进产H2O2

doi:10.1016/j.actphy.2025.100184

摘要/Abstract

摘要：

利用氧气和水光催化生产过氧化氢(H₂O₂)是一种经济环保的工艺，但开发高性能光催化剂仍具挑战性。本研究通过室温下在WO₃纳米纤维表面原位生长席夫碱聚合物三(4-氨基苯基)胺(TAPA)-对苯二甲醛(PDA)(标记为TP)，成功合成了WO₃@聚合物S型光催化剂(WO₃@TP)。所制备的WO₃@TP S型异质结展现出快速的载流子分离能力和较短的光生载流子传输距离。最优的WO₃@TP复合材料(WT-10)实现了3242 μmol g⁻¹ h⁻¹的H₂O₂产率，分别是纯WO₃和TP的137.3倍和4.6倍。通过原位辐照X射线光电子能谱(ISI-XPS)、理论计算和飞秒瞬态吸收光谱(fs-TAS)等先进表征手段的结合，验证了WO₃@TP S型异质结内的电荷转移机制。电子顺磁共振(EPR)和原位漫反射红外傅里叶变换光谱(DRIFTS)证实了反应体系中存在双通道路径(氧气还原反应(ORR)与水氧化反应(WOR))，从而促成高效H₂O₂生产。该研究不仅深化了对S型异质结中超快电荷迁移行为的理解，还为应用于太阳能驱动H₂O₂生产的无机@有机光催化剂提供了合理设计思路。

关键词: 光催化H₂O₂生成, S型异质结, 聚合物, 超快电荷转移, WO₃纳米纤维

Abstract:

Photocatalysis of H₂O₂ production using O₂ and water is a cost-effective and environmental process, but developing high-performance photocatalysts is still a challenge. Herein, a WO₃@polymer S-scheme photocatalyst was synthesized by in situ growing the Schiff-base polymer, tris-(4-aminophenyl)amine (TAPA)-terephthaldicarboxaldehyde (PDA) (labeled as TP) on the surface of WO₃ nanofibers (WO₃@TP) at room temperature. The obtained WO₃@TP S-scheme heterojunction exhibited rapid carrier separation ability and short photogenerated carriers transfer distance. The optimal WO₃@TP composite (WT-10) realized the H₂O₂ evolution rate of 3242 μmol g⁻¹ h⁻¹, which was 137.3 and 4.6-fold higher than bare WO₃ and TP, respectively. The combination of advanced characterizations regarding in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS), theoretical calculation, and femtosecond transient absorption spectroscopy (fs-TAS) validates the charge transfer mechanism within the WO₃@TP S-scheme heterojunction. The occurrence of a dual-channel pathway (O₂ reduction reaction (ORR) and water oxidation reaction (WOR) within the reaction system has been confirmed via electron paramagnetic resonance (EPR) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), thereby contributing to the highly efficient H₂O₂ evolution. This study not only gives an in-depth understanding of the ultrafast charge migration behavior in S-scheme heterojunction but also offers the rational design of inorganic@organic photocatalysts applied to solar-driven H₂O₂ production.

Key words: Photocatalytic H₂O₂ evolution, S-scheme heterojunction, Polymers, Ultrafast charge transfer, WO₃ nanofibers

朱文君, 艾陈斌, 许凯强, 周亚太, 张锡东, 张勇. WO₃@TP无机@有机S型光催化剂用于促进产H₂O₂[J]. 物理化学学报, 2026, 42(3), 100184. doi: 10.1016/j.actphy.2025.100184

Wenjun Zhu, Chenbin Ai, Kaiqiang Xu, Yatai Zhou, Xidong Zhang, Yong Zhang. WO₃@TP inorganic@organic S-scheme photocatalyst for boosting H₂O₂ production[J]. Acta Phys. -Chim. Sin. 2026, 42(3), 100184. doi: 10.1016/j.actphy.2025.100184

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100184

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I3/100184

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WO₃@TP无机@有机S型光催化剂用于促进产H₂O₂

WO₃@TP inorganic@organic S-scheme photocatalyst for boosting H₂O₂ production

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