Abstract

AbstractThe electrocatalytic sulfur reduction reaction (SRR) would allow the production of renewable high‐capacity rechargeable lithium‐sulfur (Li‐S) batteries using sustainable and nontoxic elemental sulfur as a cathode material, but its slow reaction rate causes a serious shuttle effect and dramatically reduces the capacity. We found that a catalyst composed of Pd nanoparticles supported by ordered mesoporous carbon (Pd/OMC) had a high reaction rate in the SRR, and a Li‐S battery assembled with this catalyst had a low shuttle constant of 0.031 h−1 and a high‐rate performance with a specific capacity of 1527 mAh g−1 at 0.1 C which is close to the theoretical value. The high activity of Pd/OMC with a d‐orbital vacancy of 0.87 e was predicted from a volcano relationship between the d charge for the metal and the adsorption activation entropy and reaction rate for the SRR by examining Pd, Au, Pt, Rh, and Ru transition‐metal nanocatalysts. The strategy of using a single electronic structure descriptor to design high‐efficiency SRR catalysts has suggested a way to produce practical Li‐S batteries.

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