J. Mater. Sci. Technol. ›› 2025, Vol. 206: 257-268.DOI: 10.1016/j.jmst.2024.04.028

• Research Article • Previous Articles     Next Articles

Insight into bay-/end-substituted perylene diimide and its S-scheme heterojunction for enhanced photocatalytic H2O2 production under visible-light irradiation

Bo Zhanga,b,c,d, Kang Lia,b,d, Renfu Lia,b,d, Shoufeng Wanga,b,c,d, Longtian Kanga,b,d,*   

  1. aKey Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China;
    bFujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108, China;
    cCollege of Chemistry, Fuzhou University, Fuzhou 350116, China;
    dUniversity Chinese Academy of Science, Fujian College, Fuzhou 350002, China
  • Received:2024-02-03 Revised:2024-03-26 Accepted:2024-04-14 Published:2025-01-20 Online:2025-01-20
  • Contact: *Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China. E-mail address:longtiank@fjirsm.ac.cn (L. Kang)

Abstract: Here, 1D bis(N-carboxymethyl) peryleneimide (H2PDI), 0D 1,6,7,12-tetrachloro-bis(N-carboxymethyl) peryleneimide (4Cl-H2PDI), and 2D 4Cl-H2PDI/graphene quantum dot (4Cl-H2PDI/GQD) nanostructures are synthesized and carefully analyzed. The effect of bay-/end-substitution and S-scheme heterojunction of PDI-based materials as main catalysts on the photocatalytic H2O2 evolution is first studied through the oxygen reduction reaction (ORR). Under the visible-light irradiation (> 420 nm), 4Cl-H2PDI and 4Cl-H2PDI/GQD as photocatalysts exhibit the ∼7 and ∼16 times H2O2 evolution rate than H2PDI (1059.6 vs. 2484.0 vs. 160.0 µM g-1 h-1), respectively. The systematical experiments reveal that 4Cl-H2PDI and 4Cl-H2PDI/GQD should prefer a two-step single-electron ORR process, while H2PDI may involve a 4e water oxidation and one-step 2e ORR process. Further experiments confirm that the bay-substitution and GQD doping of H2PDI can promote the generation, transportation, and separation of photogenerated electrons and holes, and prolong the carrier lifetime. This work provides insight into PDI-based photocatalytic H2O2 production.

Key words: Photocatalysis, Oxygen reduction reaction, H2O2 evolution, Perylenediimide, S-scheme heterojunction