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Optimization of photocarrier dynamics and activity in phosphorene with intrinsic defects for nitrogen fixation

Journal Article


Abstract


  • Black phosphorus has attracted ever-growing interests as an abundant and low-cost nonmetal photocatalyst for renewable energy generation. To achieve high efficiency for practical implementation, it is imperative to understand the regulation for tuning the chemical activity and meanwhile suppressing photocarrier recombination in black phosphorus. Here for the first time, we exploit the typical point defects in phosphorene to activate its basal plane and optimally modulate the photocarrier dynamics for solar-driven nitrogen reduction reaction (NRR). Combining first-principles calculations and time-dependent ab initio nonadiabatic molecular dynamics simulations, we elucidate the exact influence of each type of defect on the reduction capability and lifetime of photogenerated carriers as well as the NRR activity and selectivity of phosphorene. These results provide essential knowledge for precise design of high-efficiency nonmetal photocatalysts for hydrogen fuel storage at the atomic level.

Publication Date


  • 2020

Citation


  • Pei, W., Zhou, S., Zhao, J., Du, Y., & Dou, S. X. (2020). Optimization of photocarrier dynamics and activity in phosphorene with intrinsic defects for nitrogen fixation. Journal of Materials Chemistry A, 8(39), 20570-20580. doi:10.1039/d0ta08553g

Scopus Eid


  • 2-s2.0-85094837564

Start Page


  • 20570

End Page


  • 20580

Volume


  • 8

Issue


  • 39

Abstract


  • Black phosphorus has attracted ever-growing interests as an abundant and low-cost nonmetal photocatalyst for renewable energy generation. To achieve high efficiency for practical implementation, it is imperative to understand the regulation for tuning the chemical activity and meanwhile suppressing photocarrier recombination in black phosphorus. Here for the first time, we exploit the typical point defects in phosphorene to activate its basal plane and optimally modulate the photocarrier dynamics for solar-driven nitrogen reduction reaction (NRR). Combining first-principles calculations and time-dependent ab initio nonadiabatic molecular dynamics simulations, we elucidate the exact influence of each type of defect on the reduction capability and lifetime of photogenerated carriers as well as the NRR activity and selectivity of phosphorene. These results provide essential knowledge for precise design of high-efficiency nonmetal photocatalysts for hydrogen fuel storage at the atomic level.

Publication Date


  • 2020

Citation


  • Pei, W., Zhou, S., Zhao, J., Du, Y., & Dou, S. X. (2020). Optimization of photocarrier dynamics and activity in phosphorene with intrinsic defects for nitrogen fixation. Journal of Materials Chemistry A, 8(39), 20570-20580. doi:10.1039/d0ta08553g

Scopus Eid


  • 2-s2.0-85094837564

Start Page


  • 20570

End Page


  • 20580

Volume


  • 8

Issue


  • 39