Chinese Journal of Catalysis ›› 2025, Vol. 75: 192-203.DOI: 10.1016/S1872-2067(25)64744-9

• Article • Previous Articles    

Cobalt single atom-phosphate functionalized reduced graphene oxide/perylenetetracarboxylic acid nanosheet heterojunctions for efficiently photocatalytic H2O2 production

Wang Qihanga,1, Meng Lib,1, Li Zhuoa,*(), Yang Zhuoranb, Tang Yinana, Yu Langa, Li Zhijuna, Sun Jianhuia, Jing Liqianga,*()   

  1. aKey Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Laboratory for Catalytic Technology, Heilongjiang University, Harbin 150080, Heilongjiang, China
    bKey Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, Heilongjiang, China
  • Received:2025-03-15 Accepted:2025-04-21 Online:2025-08-18 Published:2025-07-22
  • Contact: *E-mail: lizhuo9410@hlju.edu.cn (Z. Li), jinglq@hlju.edu.cn (L. Jing).​
  • About author:1Contributed equally to this work.
  • Supported by:
    National Key R&D Program of China(2024YFF0506202);National Natural Science Foundation of China(U2102211);National Natural Science Foundation of China(U23A20576);National Natural Science Foundation of China(22402054);Outstanding Youth Science Foundation of Heilongjiang Province(YQ2024B009);Heilongjiang Province Postdoctoral Science Foundation project(LBH-Z24257);Basic Research Fund of Heilongjiang University in Heilongjiang Province(2023-KYYWF-1483)

Abstract:

The production of hydrogen peroxide (H2O2) via artificial photosynthesis using single-atom semiconductor photocatalysts represents a promising green and sustainable technology. However, its efficiency is still limited by sluggish water oxidation kinetics, poor photogenerated charge separation, and insufficient O2 adsorption and activation capabilities. Herein, uniformly dispersed single-atom catalysts (SACs) with a Co-N4 coordination structure have been synthesized by thermally transforming cobalt phthalocyanine (CoPc) assemblies pre-anchored on phosphate functionalized reduced graphene oxide (Co@rGO-P), and then used to construct heterojunctions with perylenetetracarboxylic acid (PTA) nanosheets for photocatalytic H2O2 production by an in-situ growth method. The optimized Co@rGO-P/PTA achieved an H2O2 production rate of 1.4 mmol g-1 h-1 in pure water, with a 12.9-fold enhancement compared to pristine PTA nanosheets exhibiting competitive photoactivity among reported perylene-based materials. Femtosecond transient absorption spectra, in-situ diffuse reflectance infrared Fourier transform spectra and theoretical calculations reveal that the exceptional performance is attributed to the enhanced electron transfer from PTA to rGO via the phosphate bridge and then to the Co-N4, and to the promoted O2 adsorption and activation at Co-N4 active sites. This work provides a feasible and effective strategy for designing highly efficient single-atom semiconductor heterojunction photocatalysts for H2O2 production.

Key words: Single-atom photocatalyst, Perylenetetracarboxylic acid nanosheetPhosphate-functionalized reduced, graphene oxide, Charge separation, H2O2 production