Abstract High‐energy‐density lithium–sulfur batteries exhibit obvious kinetics differences involving multistep reactions, making it hard to realize constantly high‐efficient polysulfide conversion during the full charging/discharging Herein, we propose a concept of Li + ‐respiration‐effect‐induced cascade catalysis through taking full advantage of dynamic active sites from in situ potential‐modulated TiNb 2 O 7 . The Li + respiration effect activates the lattice O atom and regulates the antibonding orbitals filling, triggering an electrochemical‐dominated switchable catalytic for sequential conversion of intermediates. As a result, the Li–S cell displays a good cycling stability and wide‐temperature ability from −30 to +60 °C. A flexible pouch cell maintains a capacity retention of 94.6% after 120 cycles. Our discovery provides a fire‐new perspective in electrochemically reconstructed catalysis for wide‐temperature‐tolerant Li − S batteries.
Zhang et al. (Tue,) studied this question.