A Metal-Free Boron Carbon Nitride (BCN) Photocatalyst for Enhanced CO2-to-CH4 Conversion by Surface Electronic Tuning

Hansong Zhang, Xinyue Han, Jingming Zhu, Siyu Lou, Pengfei Song*, Yannick J. Dappe, Zhenhuai Yang*, Yongjie Wang*, Jiaqi Zhu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Graphitic carbon nitride (g-C3N4) has emerged as an attractive metal-free photocatalyst due to its numerous advantages like tunable surface chemistry, Earth abundance, and nontoxicity. Unfortunately, its photocatalytic efficiency has been seriously limited by charge carrier recombination and low reaction dynamics. Here, we report a metal-free BCN photocatalyst achieving highly selective CO2-to-CH4 conversion under visible light without requiring any metal cocatalyst. The exfoliated CN nanosheets can enrich the reaction interface with protons to accelerate the protonation of CO intermediate to further produce CH4. Moreover, B doping not only introduces more reactive defects but also tunes its electronic structure with a more negative conduction band for rapid electron extraction and enhance CO2-to-CH4 conversion. Photocatalytic measurements show that CH4 production rate and CH4/CO ratio are 24 and 13 times higher than those of bulk CN, respectively. The CH4 production rate can also reach 130 and 31 times higher than that of few-layer g-C3N4 (FL-CN) and Cu/FL-CN, respectively. The electron selectivity toward CH4 generation on BCN photocatalysts can reach ≈90%. Furthermore, sunlight driving CO2-to-CH4 conversion on such BCN photocatalysts has also been demonstrated. This work offers new insights for the design of customized multifunctional 2D materials for solar-driven CO2 conversion to CH4.

Original languageEnglish
Article number2500037
JournalSolar RRL
Volume9
Issue number8
DOIs
Publication statusPublished - Apr 2025

Keywords

  • CH generation
  • graphitic carbon nitride
  • photocatalytic CO reduction
  • proton-coupled electron transfer
  • surface electronic tuning

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