Revealing the Rapid Electrocatalytic Behavior of Ultrafine Amorphous Defective Nb2O5x Nanocluster toward Superior LiS Performance

Abstract

The notorious shuttling behaviors and sluggish conversion kinetics of the intermediate lithium polysulfides (LPS) are hindering the practical application of lithium sulfur (Li–S) batteries. Herein, an ultrafine, amorphous, and oxygen-deficient niobium pentoxide nanocluster embedded in microporous carbon nanospheres (A-Nb2O5–x@MCS) was developed as a multifunctional sulfur immobilizer and promoter toward superior shuttle inhibition and conversion catalyzation of LPS. The A-Nb2O5–x nanocluster implanted framework uniformizes sulfur distribution, exposes vast active interfaces, and offers a reduced ion/electron transportation pathway for expedited redox reaction. Moreover, the low crystallinity feature of A-Nb2O5–x manipulates the LPS chemical affinity, while the defect chemistry enhances the intrinsic conductivity and catalytic activity for rapid electrochemical conversions. Attributed to these superiorities, A-Nb2O5–x@MCS delivers good Li–S battery performances, that is, high areal capacity of 6.62 mAh cm–2 under high sulfur loading and low electrolyte/sulfur ratio, superb rate capability, and cyclability over 1200 cycles with an ultralow capacity fading rate of 0.024% per cycle. This work provides a synergistic regulation on crystallinity and oxygen deficiency toward rapid and durable sulfur electrochemistry, holding a great promise in developing practically viable Li–S batteries and enlightening material engineering in related energy storage and conversion areas.