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

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

Abstract

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

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.

×
share this article

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)64949-2

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

Figures/Tables 11

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.

References

[1]	H. Yin Z,. Pu J,. Xue P,. Ma B,. Wu M,. Han H,. Lin Z,. Luo J,. Zeng X,. Ma H. Li, ACS Catal., 2023, 13, 7608-7615.
[2]	L. Zhou, Y. Qian, J. Chen, Y. Zhang, X. Zhou, Chem. Eng. J., 2023, 465, 142424.
[3]	X. Zheng, R. Yanagi, Z. Pan, C. Zhou, T. Liu, B. Chen, K. Katayama, S. Hu, C. Chu, Chem Catal., 2025, 5, 101238.
[4]	J. M. Campos-Martin, G. Blanco-Brieva J. L. G. Fierro, Angew. Chem. Int. Ed., 2006, 45, 6962-6984.
[5]	A. G. Fink, R. S. Delima A. R., Rousseau C,. Hunt N. E., LeSage A,. Huang M,. Stolar C. P. Berlinguette, Nat. Commun., 2024, 15, 766.
[6]	M. Sayed, H. Li, C. Bie, Acta Phys.-Chim. Sin., 2025, 41, 100117.
[7]	W. Yu, Chin. J. Catal., 2025, 73, 8-11.
[8]	A. Hayat, Z. Ajmal, A. Y. A. Alzahrani, S. Ben Moussa, M. Khered, N. Almuqati, A. Alshammari, Y. Al-Hadeethi, H. Ali, Y. Orooji, Coord. Chem. Rev., 2025, 522, 216218.
[9]	Z. Zhang, Y. Xia, C. Shao, L. Sun, G. Dawson, K. Dai, J. Mater. Sci. Technol., 2026, 252, 1-33.
[10]	X. Wang, K. Qi, K. Xu, Chin. J. Catal., 2025, 70, 1-4.
[11]	X. Zhang, D. Gao, B. Zhu, B. Cheng, J. Yu, H. Yu, Nat. Commun., 2024, 15, 3212.
[12]	H. Li W,. Wang K,. Xu B,. Cheng J,. Xu S. Cao, Chin. J. Catal., 2025, 72, 24-47.
[13]	T. Freese, J. T. Meijer, B. L. Feringa, S. B. Beil, Nat. Catal., 2023, 6, 553-558.
[14]	M. Tan Z,. Yao L,. Ma F,. Cao Y,. Peng J,. Chen Y. Bai, Coord. Chem. Rev., 2025, 544, 216993.
[15]	C. Wang, Y. Zhao, C. Cheng, Q. Li, C. Guo, Y. Hu, Coord. Chem. Rev., 2024, 521, 216177.
[16]	B. Zhu C,. Jiang J,. Xu Z,. Zhang J,. Fu J. Yu, Mater. Today, 2025, 82, 251-273.
[17]	R. He D,. Xu M,. Sayed J. Materiomics, 2025, 11, 100989.
[18]	Y. Huo X,. Zhou F,. Zhao C,. Ai Z,. Wu Z,. Chang B. Zhu, Acta Phys.-Chim. Sin., 2025, 41, 100148.
[19]	X. Liu Z. Jiang, Chin. J. Catal., 2025, 70, 5-7.
[20]	Y. Yang, X. Zhou, M. Gu, B. Cheng, Z. Wu, J. Zhang, Acta Phys.-Chim. Sin., 2025, 41, 100064.
[21]	Y. Che K,. Wang C,. Wang B,. Weng S,. Chen S,. Meng J. Mater. Sci. Technol., 2026, 243, 228-236.
[22]	X. Liu L,. Zhang W,. Jin Q,. Li Q,. Sun Y,. Wang E,. Liu X,. Hu H. Miao, Chem. Eng. J., 2023, 475, 146315.
[23]	L. Zhang, J. Zhang, J. Yu, H. García, Nat. Rev. Chem., 2025, 9, 328-342.
[24]	T. Li N,. Tsubaki Z,. Jin J. Mater. Sci. Technol., 2024, 169, 82-104.
[25]	K. Meng, J. Zhang, B. Zhu, C. Jiang, H. García, J. Yu, Adv. Mater., 2025, 37, 2505088.
[26]	G. Tang, J. Zhang, C. Bie, X. Zheng, C. Jiang, J. Yu, Adv. Mater., 2025, 37, e14576.
[27]	Y. Che B,. Weng K,. Li Z,. He S,. Chen S. Meng, Appl. Catal. B, 2025, 361, 124656.
[28]	H. Zhang, Y. Gao, S. Meng, Z. Wang, P. Wang, Z. Wang, C. Qiu, S. Chen, B. Weng, Y.-M. Zheng, Adv. Sci., 2024, 11, 2400099.
[29]	J. Jiang, J. Sun, Y. Chen, L Zhang, P. Dong. Acta Phys.-Chim. Sin. 2025, 41, 100145.
[30]	X. Wu L,. Tan G,. Chen J,. Kang G. Wang, Sci. China Mater., 2024, 67, 444-472.
[31]	P. Hao Z,. Chen Y,. Yan W,. Shi F. Guo, Sep. Purif. Technol., 2024, 330, 125302.
[32]	W. Zhong, A. Meng, Y. Su, H. Yu, P. Han, J. Yu, Angew. Chem. Int. Ed., 2025, 64, e202425038.
[33]	X. Li Z. Wang, Acta Phys.-Chim. Sin., 2025, 41, 100080.
[34]	Z. Meng, J. Zhang, H. Long, H. García, L. Zhang, B. Zhu, J. Yu, Angew. Chem. Int. Ed., 2025, 64, e202505456.
[35]	P. Shandilya, S. Sambyal, R. Sharma, P. Mandyal, B. Fang, J. Hazard. Mater., 2022, 428, 128218.
[36]	J. Fu Q,. Xu J,. Low C,. Jiang J. Yu, Appl. Catal. B, 2019, 243, 556-565.
[37]	B. Zhu J,. Sun Y,. Zhao L,. Zhang J. Yu, Adv. Mater., 2024, 36, 2310600.
[38]	X. Geng, L. Wang, L. Zhang, H. Wang, Y. Peng, Z. Bian, Chem. Eng. J., 2021, 420, 129722.
[39]	D. Liu D,. Zhang Y,. Wang E,. Liu H,. Miao J. Mater. Sci. Technol., 2024, 201, 250-260.
[40]	X. Zhou, S. Yang, X. Wang, Z. Wu, Y. Huo, J. Zhang, J. Mater. Sci. Technol., 2025, 234, 60-70.
[41]	F. Xu Y,. He J,. Zhang G,. Liang C,. Liu J. Yu, Angew. Chem. Int. Ed., 2025, 64, e202414672.
[42]	T. Wu Z,. Liu B,. Shao Q,. Liang Q,. He Y,. Pan X,. Zhang Y,. Liu J,. Sun S. Gong, Chem. Eng. J., 2022, 447, 137332.
[43]	J. Yue H,. Yang S,. Wang C,. Liu L,. Wang J. Colloid Interface Sci., 2024, 653, 981-991.
[44]	X. Zhang, W. Ni, X. Yue, Z. Wang, Z. Zhang, K. Wang, W. Dai, X. Fu, J. Colloid Interface Sci., 2025, 678, 233-245.
[45]	T. G. Novak, J. Kim P. A., DeSario S. Jeon, Nanoscale Adv., 2021, 3, 5166-5182.
[46]	X. Wu M,. Sayed G,. Wang W,. Yu B. Zhu, Adv. Mater., 2025, DOI: 10.1002/adma.202511322.
[47]	Y. Ma S,. Wang Y,. Zhang B,. Cheng L,. Zhang J. Materiomics, 2025, 11, 100978.
[48]	B. Liu J,. Zhang H,. Li B,. Cheng C. Bie, Acta Phys. -Chim. Sin., 2025, 41, 100121.
[49]	L. Wang, J. Zhao, J. Mater. Sci. Technol., 2026, 241, 18-20.
[50]	F. A. Qaraah, S. A. Mahyoub, A. Hezam, A. Qaraah, F. Xin, G. Xiu, Appl. Catal. B, 2022, 315, 121585.
[51]	S. Li R,. Li K,. Dong Y,. Liu X,. Yu W,. Li T,. Liu Z,. Zhao M,. Zhang B,. Zhang X. Chen, Chin. J. Catal., 2025, 76, 37-49.
[52]	Z. Liu F,. Jin X,. Li P,. Zhang Z,. Jin J. Mater. Sci. Technol., 2024, 188, 131-143.
[53]	Y. Zhang, J. Pan, X. Ni, F. Mo, Y. Xu, P. Dong, Chin. J. Catal., 2025, 74, 250-263.
[54]	M. Sayed, K. Qi, X. Wu, L. Zhang, H. García, J. Yu, Chem. Soc. Rev., 2025, 54, 4874-4921.
[55]	M. Gu J,. Zhang I. V., Kurganskii A. S., Poryvaev M. V., Fedin B,. Cheng J,. Yu L. Zhang, Adv. Mater., 2025, 37, 2414803.
[56]	X. Yin J,. Yu H. Yu, J. Am. Chem. Soc., 2025, 147, 34881-34890.
[57]	Z. Jiang, J. Zhang, B. Cheng, Y. Zhang, J. Yu, L. Zhang, Small, 2025, 21, 2409079.
[58]	X. Zhou, Y. Huo. S. Yang, B. He, X. Wang, Z. Wu, J. Zhang, Acta Phys. -Chim. Sin. 2025, 41, 100160.
[59]	D. Xu R,. He Z,. Jiang J. Mater. Sci. Technol., 2025, 236, 280-283.
[60]	J. Qiu C,. Cheng H,. García G,. Liang B,. Zhu L,. Zhang J. Yu, Angew. Chem. Int. Ed., 2025, 64, e202515898.
[61]	F. Fu Y. Li, Chin. J. Catal., 2025, 78, 4-6.
[62]	Y. Zhou, P. Dong, J. Liu, B. Zhang, B. Zhang, X. Xi, J. Zhang, Adv. Funct. Mater., 2025, 35, 2500733.
[63]	J. Du Y,. Shen L,. Yan H,. Miao X. Hou, Sep. Purif. Technol., 2026, 380, 135331.
[64]	M. Li X,. Li J. B. Ghasemi, Chin. J. Catal., 2025, 73, 12-15.
[65]	C. Cheng, J. Yu, D. Xu, L. Wang, G. Liang, L. Zhang, M. Jaroniec, Nat. Commun., 2024, 15, 1313.
[66]	M. Gu Y,. Yang B,. Cheng L,. Zhang P,. Xiao T. Chen, Chin. J. Catal., 2024, 59, 185-194.
[67]	J. Pan A,. Zhang L,. Zhang P. Dong, Chin. J. Catal., 2024, 58, 180-193.
[68]	K. Meng, J. Zhang, B. Cheng, X. Ren, Z. Xia, F. Xu, L. Zhang, J. Yu, Adv. Mater., 2024, 36, 2406460.
[69]	Y. Wu Y,. Yang M,. Gu C,. Bie H,. Tan B,. Cheng J. Xu, Chin. J. Catal., 2023, 53, 123-133.
[70]	Y. Zhang, Y. Wang, Y. Liu, S. Zhang, Y. Zhao, J. Zhang, J. Materiomics, 2025, 11, 100985.
[71]	Y. Liu M,. Li T,. Liu Z,. Wu L,. Zhang J. Mater. Sci. Technol., 2025, 233, 201-209.
[72]	C. Jiang, C. Yuan, K. Xu, X. Zhou, C. Bie, J. Mater. Sci. Technol., 2025, 231, 36-44.
[73]	K. Li J,. Mei J,. Li Y,. Liu G,. Wang D,. Hu S,. Yan K. Wang, Sci. China Mater., 2024, 67, 484-492.
[74]	X. Zhou, C. Ai, X. Wang, Z. Wu, J. Zhang, J. Materiomics, 2025, 11, 100974.
[75]	Y. Zhang, J. Qiu, B. Zhu, G. Sun, B. Cheng, L. Wang, Chin. J. Catal., 2024, 57, 143-153.

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

RichHTML

PDF (PC)

Knowledge

Supporting Information

Abstract

Cite this article

share this article

share this article

Figures/Tables 11

References

Related Articles 15

Recommended Articles

Metrics

[1]	Yuhang Sun, Xu Li, Zhongtian Zeng, Hua Wei, Yulong Zhao, Xiaoyan Cai, Liang Mao, Chang-Long Tan, Bo Shen, Yi-Jun Xu. Sulfur-induced charge-site reconstruction and in-situ formed ZnO₂ protection enable robust solar H₂O₂production [J]. Chinese Journal of Catalysis, 2026, 88(9): 207-217.
[2]	Xiaolong Ma, Zhiqiang Wu, Huiqin Yao, Bin Liu, Zhiliang Jin, Paolo Fornasiero. Charging dynamics engineering: Quantum dots-induced full-space electric field cooperative Ag₂S QDs/CoWO₄ S-scheme heterojunction boosting photocatalytic hydrogen evolution [J]. Chinese Journal of Catalysis, 2026, 88(9): 233-246.
[3]	Gaoxiong Liu, Rundong Chen, Bingquan Xia, Xianlong Zhou, Laiquan Li, Shantang Liu. Thiadiazole-functionalized covalent triazine frameworks for constructing S-scheme heterojunctions enabling boosted H₂O₂ photosynthesis [J]. Chinese Journal of Catalysis, 2026, 87(8): 170-184.
[4]	Hao Wu, Xinyu Zeng, Wang Wang, Bei Cheng, Jingzhao Cheng, Jingsan Xu, Shaowen Cao. The organic-inorganic S-scheme heterojunction with enhanced charge separation simultaneously catalyze the production of hydrogen and imine [J]. Chinese Journal of Catalysis, 2026, 87(8): 185-196.
[5]	Sue-Faye Ng, Joel Jie Foo, Karlo Nolkemper, Zahra Hajiahmadi, Jaya Bharti, Nannan Hou, Jiankang Zheng, Thomas D. Kühne, Markus Antonietti, Christian Mark Pelicano, Wee-Jun Ong. Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H₂O₂ synthesis [J]. Chinese Journal of Catalysis, 2026, 87(8): 140-155.
[6]	Shijie Li, Rui Li, Yanping Liu, Xin Yu, Deyun Ma, Jianhui Jiang, Xiaosong Zhou, Chunqiang Zhuang, Zaiwang Zhao, Wei Jiang. Augmented reactive oxygen species generation in Ag/AgBr/C₃N₅ via LSPR-enhanced S-scheme charge transfer for efficient photocatalytic antibiotic wastewater remediation [J]. Chinese Journal of Catalysis, 2026, 87(8): 126-139.
[7]	Ke Li, Yi Luo, Chenning Cai, Zemin Zheng, Gang Yu, Jianqiang Hu, Shengli Chen. WN enhanced metal-N-C platform for ultra-stable Pt oxygen reduction electrocatalyst in fuel cell [J]. Chinese Journal of Catalysis, 2026, 87(8): 230-242.
[8]	Yatai Zhou, Chengcheng Yuan, Wei Xia, Jun Wang, Xiaofeng Zhu, Yong Zhang, Bicheng Zhu, Jiaguo Yu. Synergistic optimization of interfacial electron transfer and surface hydrogen adsorption in a CdS/ZnO S-scheme heterojunction by site-specific doping: A DFT study [J]. Chinese Journal of Catalysis, 2026, 86(7): 327-337.
[9]	Xiang Wang, Min Zhou, Xiaobin Liao, Xu Han, Congcong Xing, René Bes, Simo Huotari, Jordi Arbiol, Andreu Cabot. Enhanced oxygen evolution and reduction by phosphorus-doped Co₉S₈ derived from MOFs: Toward high-performance zinc-air batteries [J]. Chinese Journal of Catalysis, 2026, 85(6): 204-215.
[10]	Jintao Dong, Rui Zhang, Zhishuai Wang, Shengqun Cao, Lina Li, Gaopeng Liu, Bin Wang, Yixuan Gao, Jiexiang Xia. Construction of S-scheme MnO₂/BiOCl heterojunction boosting photocatalytic low-concentration peroxymonosulfate activation for contaminants removal [J]. Chinese Journal of Catalysis, 2026, 85(6): 310-321.
[11]	Qianqian Xu, Haihong Zhong, Chunli Li, Rong Jiang, Yongjun Feng, Luis Alberto Estudillo-Wong. O-bridged NiSe₂/CQDs composite synergistically triggers interfacial electrons transfer to promote H₂O₂ electrosynthesis [J]. Chinese Journal of Catalysis, 2026, 85(6): 258-271.
[12]	Wenning Liu, Li An, Jinming Wang, Ruyue Li, Jie Mu, Yongde Long, Dan Qu, Yichang Liu, Yuxiang Hu, Xiayan Wang, Ning Jiang, Zaicheng Sun. Group IIIA metals-induced p-d orbital hybridization enhances the oxygen reduction performance of Pd based metallene in zinc-air batteries [J]. Chinese Journal of Catalysis, 2026, 84(5): 144-158.
[13]	Ran Sun, Yuqi Zhang, Kunge Hou, Yujie Tan, Xingang Liu, Jianyuan Hou, Weixuan Zhao, Andrew E. H. Wheatley, Renxi Zhang. Designing hydrogen-bonds in covalent organic frameworks: accelerating proton-coupled electron transfer for enhanced photocatalytic H₂O₂ synthesis [J]. Chinese Journal of Catalysis, 2026, 84(5): 274-287.
[14]	Yong Zhang, Wenjun Zhu, Yanyan Zhao, Shumin Zhang. In₂S₃/HOF S-scheme heterojunction for enhanced photocatalytic H₂O₂ production [J]. Chinese Journal of Catalysis, 2026, 84(5): 261-273.
[15]	Ziyi Liao, Lan Jiang, Yang Yang, Lin Wang, Weiyou Yang, Huilin Hou. Alkali-cyano dual-tailored g-C₃N₄/BiOCl S-scheme heterojunctions for highly efficient visible-light-driven H₂O₂ photosynthesis in pure water [J]. Chinese Journal of Catalysis, 2026, 83(4): 143-161.