| Summary: | Abstract The viability of lithium‐sulfur (Li–S) batteries toward real implementation directly correlates with unlocking lithium polysulfide (LiPS) evolution reactions. Along this line, designing promotors with the function of synchronously relieving LiPS shuttle and promoting sulfur conversion is critical. Herein, the nitrogen evolution on hierarchical and atomistic Ni–N–C electrocatalyst, mainly pertaining to the essential subtraction, reservation and coordination of nitrogen atoms, is manipulated to attain favorable Li–S pouch cell performances. Such rational evolution behavior realizes the “nitrogen balance” in simultaneously regulating the Ni–N coordination environment, Ni single atom loading, abundant vacancy defects, active nitrogen and electron conductivity, and maximizing the electrocatalytic activity elevation of Ni–N–C system. With such merit, the cathode harvests favorable performances in a soft‐packaged pouch cell prototype even under high sulfur mass loading and lean electrolyte usage. A specific energy density up to 405.1 Wh kg−1 is harvested by the 0.5‐Ah‐level pouch cell.
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