二维/二维g-C3N4/WO3 S型异质结中的超快电子转移及其高效光催化产H2O2机理

doi:10.1016/S1872-2067(26)64949-2

催化学报 ›› 2026, Vol. 85: 333-345.DOI: 10.1016/S1872-2067(26)64949-2

二维/二维g-C₃N₄/WO₃ S型异质结中的超快电子转移及其高效光催化产H₂O₂机理

李萍^a, 韦良^a, 夏伟^b, 袁成成^c, 艾陈斌^c, 李猛^a()

^a 南宁师范大学广西天然高分子化学与物理重点实验室, 广西南宁 530001
^b 茅台学院资源与环境学院, 贵州仁怀 564507
^c 中国地质大学(武汉)材料与化学学院, 太阳燃料实验室, 湖北武汉 430078

收稿日期:2025-10-06 接受日期:2025-11-09 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: limeng_2016@126.com (李猛).
基金资助:
国家自然科学基金(42207386);广西自然科学基金(2025GXNSFBA069543);茅台学院酒产业研究院专项课题(MTXYJCY002)

Ultrafast electron transfer in 2D/2D g-C₃N₄/WO₃ S-scheme heterojunctions for enhanced H₂O₂ production

Ping Li^a, Liang Wei^a, Wei Xia^b, Chengcheng Yuan^c, Chenbin Ai^c, Meng Li^a()

^a Guangxi Key Laboratory of Natural Polymer Chemistry and Physics, Nanning Normal University, Nanning 530001, Guangxi, China
^b School of Resources and Environment Engineering, Moutai Institute, Renhuai 564507, Guizhou, China
^c Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei, China

Received:2025-10-06 Accepted:2025-11-09 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: limeng_2016@126.com (M. Li).
Supported by:
National Natural Science Foundation of China(42207386);Natural Science Foundation of Guangxi Autonomous Region(2025GXNSFBA069543);Special Project of the Liquor Industry Research Center of Moutai Institute(MTXYJCY002)

摘要/Abstract

摘要：

过氧化氢(H₂O₂)作为重要的化工原料和环保产品, 在化学合成、环境治理和能量存储等领域具有重要应用. 传统的蒽醌氧化工艺在H₂O₂制备中存在能耗高、依赖化石资源、污染严重等问题. 因此, 开发绿色、高效的H₂O₂合成方法已成为当今科学研究的重要课题. 光催化制H₂O₂通过氧还原反应(ORR)或水氧化反应(WOR)在常温常压下进行, 利用太阳能驱动, 发展具有可持续性. 然而, 当前光催化过程面临光生电子-空穴复合快、竞争性副反应多等严峻挑战. 因此, 设计具有强氧化还原能力和高效电荷分离性能的光催化剂是实现高效产H₂O₂的关键.

本文采用创新的异质结设计策略, 通过原位水热生长法制备了二维/二维g-C₃N₄/WO₃ S型异质结光催化剂. 该设计充分利用g-C₃N₄还原能力强与WO₃价氧化能力强的特点, 构建了一个具有原子级紧密界面的S型异质结体系. 在该异质结中, 内建电场的建立可以驱使光生电荷按照S型机制定向转移, 实现低能量载流子在界面处的有效复合, 同时保留高能量电子和空穴, 使其分别用于高效的O₂还原和乙醇氧化反应. 系统的表征手段证实了S型异质结的形成. X-射线衍射、红外光谱和透射电镜等表征证实了g-C₃N₄与WO₃紧密结合, 并保留各自的层状结构与晶相. 光学与电化学分析表明, g-C₃N₄和WO₃之间形成了典型的S型能带结构, 且载流子复合显著抑制, 分离与转移效率大幅提高. 原位X-射线光电子能谱分析表明, 在暗条件及照射下探测到C 1s, N 1s与W 4f, O 1s峰的相反偏移, 证实了界面内建电场的形成以及光激发下WO₃中的光生电子转移至g-C₃N₄; 开尔文探针力显微镜清晰显示了光照前后催化剂表面电势分布, 证实了光生电子从WO₃向g-C₃N₄转移; 密度泛函理论计算证实了异质结界面处0.47 e从g-C₃N₄迁移至WO₃建立内建电场. 飞秒瞬态吸收光谱直接捕捉界面电子转移过程, g-C₃N₄/WO₃复合物中WO₃导带电子在约46.1 ps内与g-C₃N₄价带空穴的界面复合. 优化的CW15异质结样品在光照射下表现出优异的H₂O₂生成性能, 产率达到2571.6 μmol g^-1 h^-1, 分别是纯g-C₃N₄和WO₃的2.8倍和63.5倍, 光催化循环实验证明CW15异质结具有优异的化学和结构稳定性. 自由基捕获实验、电子顺磁共振和原位漫反射傅里叶变换红外光谱研究揭示了反应机理: O₂通过单电子逐步氧还原过程(O₂ + e^- → ·O₂^-, 2H⁺ + ·O₂^- + e^- → H₂O₂)生成H₂O₂, 而乙醇作为空穴牺牲剂被逐步氧化.

综上, 本研究成功构建了二维/二维g-C₃N₄/WO₃ S型异质结, 并揭示了其超快电子转移与高效H₂O₂生成机制, 对进一步设计高效光催化氧还原体系具有指导意义. 该策略未来可推广到其他光响应半导体组合, 为清洁能源转化与绿色化学提供可扩展的材料体系.

关键词: g-C₃N₄, WO₃, S型异质结, 产H₂O₂, 氧还原反应

Abstract:

The increasing demand for sustainable and environmentally friendly hydrogen peroxide (H₂O₂) production has necessitated the development of efficient photocatalytic strategies. A two-dimensional (2D)/2D graphitic carbon nitride (g-C₃N₄)/WO₃ S-scheme heterojunction was synthesized in this study via in situ growth, yielding an atomically intimate interface that promotes ultrafast interfacial charge transfer. Comprehensive spectroscopy, photoelectrochemistry, Kelvin probe force microscopy, and density functional theory investigations confirmed the S-scheme charge-transfer mechanism. This system, driven by an internal electric field, promotes the spatial separation of photoexcited charge carriers and maintains robust redox abilities. Femtosecond transient absorption spectroscopy revealed ultrafast interfacial charge transfer from WO₃ to g-C₃N₄. The optimized heterostructure exhibited considerably photocatalytic activity, achieving a 2571.6 μmol g⁻¹ h⁻¹ H₂O₂ production rate, representing 2.8- and 63.5-fold improvements over g-C₃N₄ and WO₃, respectively. Electron paramagnetic resonance and in situ diffuse reflectance infrared Fourier-transform spectroscopy were used to elucidate the oxygen reduction reaction mechanism, indicating that ethanol undergoes sequential oxidation, whereas photogenerated electrons reduce O₂ to produce H₂O₂ through a sequential single-electron process. This study offers significant mechanistic insights into the carrier dynamics within 2D S-scheme heterojunctions and presents a scalable and efficient route for green H₂O₂ synthesis.

Key words: g-C₃N₄, WO₃, S-scheme heterojunction, H₂O₂ production, Oxygen reduction reaction

李萍, 韦良, 夏伟, 袁成成, 艾陈斌, 李猛. 二维/二维g-C₃N₄/WO₃ S型异质结中的超快电子转移及其高效光催化产H₂O₂机理[J]. 催化学报, 2026, 85: 333-345.

Ping Li, Liang Wei, Wei Xia, Chengcheng Yuan, Chenbin Ai, Meng Li. Ultrafast electron transfer in 2D/2D g-C₃N₄/WO₃ S-scheme heterojunctions for enhanced H₂O₂ production[J]. Chinese Journal of Catalysis, 2026, 85: 333-345.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)64949-2

https://www.cjcatal.com/CN/Y2026/V85/I6/333

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Fig. 1. (a) Schematic diagram illustrating the synthesis of the 2D/2D g-C3N4/WO3 heterostructures. XRD patterns (b) and FTIR spectra (c) of pure g-C3N4, WO3, and their composites.

Fig. 2. FESEM images of g-C3N4 (a), WO3 nanosheets (b), and CW15 (c). TEM (d) and HRTEM (e) images of CW15. HAADF image (f) and corresponding EDX elemental maps (g-j) of CW15, confirming the homogeneous distribution of C, N, W, and O.

Fig. 3. (a) UV-vis DRS spectra of pure g-C3N4, WO3, and their composites. Tauc plot analysis (b), Mott-Schottky electrochemical plots (c), and schematic diagram illustrating the electronic band structure (d) for g-C3N4 and WO3.

Fig. 4. PL spectra (a), TRPL decay profiles (b), transient photocurrent densities (c), and EIS Nyquist plots (d) of g-C3N4, WO3, and their composites.

Fig. 5. High-resolution XPS spectra for the C 1s (a), N 1s (b), W 4f (c), and O 1s (d) regions of g-C3N4, WO3, and CW15 under dark and light irradiation.

Fig. 6. EPR spectra for DMPO-·O2- (a) and DMPO-·OH (b) for g-C3N4, WO3 and CW15.

Fig. 7. KPFM images of CW15 in the dark (a) and under light illumination (b). Corresponding VCPD (c) and SPV (d) of CW15 along the marked line.

Fig. 8. Calculated electrostatic potentials of the g-C3N4 (001) (a) and WO3 (001) (b) slabs. (c) Charge density difference of the g-C3N4/WO3 heterojunction interface; cyan and yellow isosurfaces represent electron depletion and accumulation regions, respectively. (d) Schematic diagram illustrating the interfacial electron transfer pathways and IEF formation in the S-scheme heterojunction.

Fig. 9. Two-dimensional pseudocolor fs-TA spectral maps for g-C3N4 (a), WO3 (b) and CW15 (c). Normalized temporal decay profiles of the GSB signals for g-C3N4 and CW15 probed at 430 nm (d) and WO3 probed at 420 nm within 6000 ps (e). (f) Schematic diagram illustrating the mechanistic pathways for photogenerated carrier relaxation and the charge transfer dynamics within the g-C3N4/WO3 S-scheme heterojunction.

Fig. 10. (a) Time-dependent photocatalytic H2O2 production over the as-prepared samples using ethanol as a sacrificial agent. (b) Comparison of the H2O2 production rates for the as-prepared samples. (c) Photocatalytic decomposition kinetics of 1 mmol L-1 H2O2 under light irradiation for 60 min. (d) Kinetic constants for H2O2 formation and decomposition derived from the data in (a) and (c).

Fig. 11. (a) Photocatalytic H2O2 production by CW15 in an N2 atmosphere, pure water, and various trapping agents. (b) Pseudocolor map depicting the temporal spectral intensity evolution on CW15 during dark adsorption and subsequent light irradiation with a H2O, O2, and ethanol mixed gas flow, followed by light irradiation. (c) Representative in-situ DRIFTS spectra of CW15.

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二维/二维g-C₃N₄/WO₃ S型异质结中的超快电子转移及其高效光催化产H₂O₂机理

Ultrafast electron transfer in 2D/2D g-C₃N₄/WO₃ S-scheme heterojunctions for enhanced H₂O₂ production

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