Facilitating carrier kinetics in ultrathin porous carbon nitride through shear-repair strategy for peroxymonosulfate-assisted water purification

Hao Liu; Bin Yang; Guangfu Liao; Baoyu Huang; Jun Li; Raul D Rodriguez; Xin Jia

doi:10.1038/s41467-025-61185-3

Facilitating carrier kinetics in ultrathin porous carbon nitride through shear-repair strategy for peroxymonosulfate-assisted water purification

Nat Commun. 2025 Jul 1;16(1):5909. doi: 10.1038/s41467-025-61185-3.

Authors

Hao Liu^#¹, Bin Yang^#², Guangfu Liao³, Baoyu Huang⁴, Jun Li⁵, Raul D Rodriguez⁶, Xin Jia⁷

Affiliations

¹ School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi, China.
² School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi, China. yangbin@shzu.edu.cn.
³ College of Material Engineering, Fujian Agriculture and Forestry University, Fuzhou, P. R. China.
⁴ Hunan Provincial Key Laboratory of Environmental Catalysis & Waste Recycling, College of Materials and Chemical Engineering, Hunan Institute of Engineering, Xiangtan, China.
⁵ School of Chemical Engineering, Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou, P.R. China. junli2019@zzu.edu.cn.
⁶ Tomsk Polytechnic University, 30 Lenin Avenue, Tomsk, Russia.
⁷ School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, Shihezi University, Shihezi, China. jiaxin@shzu.edu.cn.

^# Contributed equally.

Abstract

Achieving high specific surface area (HSSA) in graphitic carbon nitride (g-C₃N₄) severely depolymerizes the molecular chain structure, resulting in sluggish carrier kinetic behaviors and thus moderated water purification performance in photocatalytic peroxymonosulfate (PMS) activation system. Herein, we report a versatile shear-repair strategy for fabricating ultrathin porous g-C₃N₄ nanosheets with a thickness of 1.5 nm, HSSA (138.5 m² g^-1), and highly polymerized molecular chains. This strategy accelerates exciton dissociation and charge carrier separation, with the exciton binding energy decreasing from 65.7 to 47.5 meV. Crucially, the electron-donating pollutant and electron-withdrawing PMS generate a microelectric field at the g-C₃N₄ surface that activates PMS to generate ¹O₂ sustainably. Consequently, our catalyst exhibits an exceptional imidacloprid (IMD) removal performance with a rate constant of 0.405 min^-1 and remarkable PMS utilization efficiency (90% within 15 min). Moreover, under real conditions of sunlight irradiation, we observe an outstanding pollutants' removal efficiency with a near-100% degradation rate over 20 days of continuous operation. Our work emphasizes the feasibility of synergistic molecular-level structural engineering for refining carrier kinetic behaviors in high-performance photocatalyst design.

Abstract

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