Acta Phys. -Chim. Sin. ›› 2024, Vol. 40 ›› Issue (11): 2406005.doi: 10.3866/PKU.WHXB202406005

Special Issue: Solar fuel preparation

• ARTICLE • Previous Articles     Next Articles

Simultaneously Improving Inter-Plane Crystallization and Incorporating K Atoms in g-C3N4 Photocatalyst for Highly-Efficient H2O2 Photosynthesis

Wei Zhong, Dan Zheng, Yuanxin Ou, Aiyun Meng*(), Yaorong Su*()   

  1. College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, Guangdong Province, China
  • Received:2024-06-05 Revised:2024-07-16 Accepted:2024-07-17 Published:2024-10-14
  • Contact: Email: mengaiyun@sztu.edu.cn (Aiyun Meng)suyaorong@sztu.edu.cn; Tel: +86-755-2325-6080 (Yaorong Su)
  • Supported by:
    the National Natural Science Foundation of China(22178224); the National Natural Science Foundation of China(22272110); Guangdong Basic and Applied Basic Research Foundation(2023A1515110535); Guangdong Basic and Applied Basic Research Foundation(2020A1515110873); Shenzhen Science and Technology Program(RCBS20231211090522041); the Fundamental Research Funds for Shenzhen Technology University(20211063010047); Shenzhen Key Laboratory of Applied Technologies of Super-Diamond and Functional Crystals(ZDSYS20230626091303007); Shenzhen Science and Technology Program(20231127203830001)

Abstract:

Graphitic carbon nitride (g-C3N4) has gained growing attention in hydrogen peroxide (H2O2) photosynthesis, but the low activity of two-electron oxygen reduction reaction (2e--ORR) still restricts its photocatalytic H2O2-generation performance. Herein, traditional g-C3N4 photocatalysts are recrystallized on KI crystal surfaces by a secondary calcination route to synthesize K incorporated highly-crystalline g-C3N4 photocatalysts. The synthesized CN-K photocatalyst exhibits improved inter-plane crystallization, narrowed bandgap structure, and smaller particle size from 20 to 50 nm. Moreover, the incorporated K atoms, as excellent catalytic sites, can enhance O2 adsorption and stabilize the *OOH intermediates, thus improving the 2e--ORR activity of the K incorporated high-crystallization g-C3N4 photocatalysts. Consequently, the optimized CN-K(1:6) photocatalyst exhibits a remarkably improved H2O2-generation rate of 7.8 mmol·L-1·h-1 with an AQE value of 5.17% at 420 nm, outperforming the traditional g-C3N4 sample by a factor of 220. This work uncovers the roles of heteroatoms in promoting the 2e--ORR selectivity of the g-C3N4 photocatalyst, and offers novel insights to construct highly-active g-C3N4-based materials for H2O2 photosynthesis.

Key words: Photocatalytic H2O2 evolution, Carbon nitride, K incorporation, Highly-selective 2e--ORR