Dynamic Ni–N 4 centers enable concurrent polysulfide catalysis and Li + flux control for high‐performance Li–S batteries

Abstract This work introduces nickel (II) tetraphenylporphyrin (NiTPP) as a multifunctional electrolyte additive to simultaneously address polysulfide shuttle and uncontrolled lithium dendrite growth in lithium–sulfur (Li–S) batteries. Mobile NiTPP species act as homogeneous catalysts with Ni–N 4 centers for rapid polysulfide redox mediation to suppress migration, while planar molecules featuring lithium‐affinity capability migrate to the lithium metal surfaces, enabling uniform lithium flux and anode protection. NiTPP‐modified electrolytes significantly enhance Li–S battery performance, demonstrated by 634.9 mAh g −1 at 4C, 758.3 mAh g −1 after 100 cycles at 0.2 C (83.4% retention), and 757.5 mAh g −1 under…

• NN
  National Natural Science Foundation of China

  Award: 22263009