Fluorine-Stabilized Defective Black Phosphorene as a Lithium-Like Catalyst for Boosting Nitrogen Electroreduction to Ammonia

作者：Liu, Honghong; Hai, Guangtong; Ding, Liang-Xin^*; Wang, Haihui^*

来源：Angewandte Chemie - International Edition, 2023.

DOI：10.1002/anie.202302124

• Ammonia Synthesis
• Black Phosphorene
• Defect Engineering
• Lithium-Like Catalyst
• Nitrogen Reduction Reaction

Electrocatalytic N-2 reduction reaction (NRR) is recognized as a zero-carbon emission method for NH3 synthesis. However, to date, this technology still suffers from low yield and low selectivity associated with the catalyst. Herein, inspired by the activation of N-2 by lithium metal, a highly reactive defective black phosphorene (D-BPene) is proposed as a lithium-like catalyst for boosting electrochemical N-2 activation. Correspondingly, we also report a strategy for producing environmentally stable D-BPene by simultaneously constructing defects and fluorination protection based on topochemical reactions. Reliable performance evaluations show that the fluorine-stabilized D-BPene can induce a high NH3 yield rate of approximate to 70 mu g h(-1) mg(cat.)(-1) and a high Faradaic efficiency of approximate to 26 % at -0.5 V vs. RHE in an aqueous electrolyte. This work not only exemplifies the first stable preparation and practical application of D-BPene, but also brings a new design idea for NRR catalysts.

• 单位
  清华大学