Journal
SMALL METHODS
Volume 4, Issue 6, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.201900344
Keywords
electrocatalysis; lithium sulfide nucleation; lithium-sulfur batteries; polysulfide redox reaction; redox mediator
Funding
- National Key Research and Development Program [2016YFA0202500, 2016YFA0200102]
- National Natural Science Foundation of China [21776019, 21825501, U1801257]
- Beijing Key Research and Development Plan [Z181100004518001]
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Regulating the solid product growth is critical for achieving high capacities in rechargeable batteries based upon multiphase and multielectron dissolution-precipitation chemistries (e.g., lithium-sulfur chemistry). The intrinsic redox mediators, polysulfides, are insufficient for effective regulation due to the dynamically changed species and concentration. Herein cobaltocene (CoCp2) is introduced as a persistent extrinsic redox mediator to dictate an alternative growing pathway toward three-dimensional lithium sulfide growth, which enables at most 8.1 times enhancement in discharge capacities at harsh conditions of high-rate (>1 C) or electrolyte-lean operation (electrolyte/sulfur ratio of 4.7 mu L mg(S)(-1)). The faster kinetics and higher diffusivity of CoCp2 play an essential role in regulating lithium sulfide growth and increasing discharge capacities. This work not only illustrates an effective strategy to increase the capacity of high-rate or electrolyte-lean lithium-sulfur batteries but also paves a way toward the rational design of novel redox mediators for dissolution-precipitation energy chemistries.
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