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Electrocatalytic N2 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 N2 by lithium metal, a highly reactive defective black phosphorene (D−BPene) is proposed as a lithium‐like catalyst for boosting electrochemical...