Chinese Journal of Catalysis ›› 2026, Vol. 87: 140-155.DOI: 10.1016/S1872-2067(26)65093-0

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Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H2O2 synthesis

Sue-Faye Nga,b,c, Joel Jie Fooa,b, Karlo Nolkemperc,d,e, Zahra Hajiahmadid,e, Jaya Bhartic, Nannan Houg, Jiankang Zhengg, Thomas D. Kühned,e,f, Markus Antoniettic, Christian Mark Pelicanoc,*(), Wee-Jun Onga,b,h,i,*()   

  1. a School of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
    b Center of Excellence for NaNo Energy & Catalysis Technology (CONNECT), Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
    c Department of Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, Potsdam 14476, Germany
    d Center for Advanced Systems Understanding (CASUS), Untermarkt 20, 02826 Görlitz, Germany
    e Helmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstrasse 400, 01328 Dresden, Germany
    f Institute of Artificial Intelligence, Chair of Computational System Sciences, Technische Universitat Dresden, 01187 Dresden, Germany
    g CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei 230026, Anhui, China
    h State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
    i Gulei Innovation Institute, Xiamen University, Zhangzhou 363200, Fujian, China
    j Shenzhen Research Institute of Xiamen University, Shenzhen 518057, Guangdong, China
    k Department of Chemical and Biological Engineering, College of Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul 02841, Republic of Korea
  • Received:2025-09-19 Accepted:2026-01-12 Online:2026-08-05 Published:2026-06-24
  • Supported by:
    National Natural Science Foundation of China(22202168);Guangdong Basic and Applied Basic Research Foundation(2021A1515111019);Embassy of the People’s Republic of China in Malaysia(EENG/0045);State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University(2023X11);Xiamen University Malaysia Investigatorship(IENG/0038);Xiamen University Malaysia Research Fund(ICOE/0001);Xiamen University Malaysia Research Fund(IENG/0090);Xiamen University Malaysia Research Fund(XMUMRF/2021-C8/IENG/0041);Xiamen University Malaysia Research Fund(XMUMRF/2025-C15/IENG/0080)

Abstract:

Light-driven synthesis of hydrogen peroxide (H2O2) presents an ideal pathway for sustainability as compared to the traditional anthraquinone process. Herein, we introduce a strategic approach for functionalizing poly(heptazine imide) with triazole groups via a one-step calcination process using alkali-metal salts (NaCl/KCl/LiCl). Featuring a donor-acceptor framework that promotes singlet electron dissociation, the optimal catalyst (KNa) displayed outstanding photocatalytic performance, achieving H2O2 production at 9.32 mmol L-1 h-1 and benzaldehyde (BAD) generation at 8.14 mmol L-1 h-1. KNa reached an apparent quantum efficiency of 11.58% at 420 nm, in the absence of noble-metal cocatalysts. It also exhibited an electron-hole utilization close to unity (89%), indicating its efficiency in driving photoredox reactions. Mechanistic studies conducted through electrochemical measurements and scavenger tests revealed that KNa facilitated a 2-electron pathway for H2O2 production, with photogenerated charges and radicals (electron, hole, O2•-, 1O2) participating in the reaction. A shift in electron density and enhanced O2 adsorption observed from computational analysis reflects the donor-acceptor effect of the terminal triazole units on PHI. The versatility of KNa for other photochemical reactions was also exemplified by its simultaneous generation of H2O2 (1.11 mmol L-1 h-1) and furfuraldehyde (0.75 mmol L-1 h-1). As such, this research paves an in-depth understanding of synergistic dual-functional photocatalysts for photoredox reactions.

Key words: Carbon nitride, Photocatalyst, Electron-hole utilization, H2O2 production, Benzaldehyde production