Nitrogen-doped carbon nanofiber loaded MOF-derived NiCo bimetallic nanoparticles accelerate the redox transformation of polysulfide for lithium- sulfur batteries

Abstract

In the electrochemical study of lithium-sulfur (Li-S) batteries, the slow kinetics of the sulfur reduction reaction (SRR) leading to severe shuttle effect of polysulfides remains a major challenge. Catalysts with bimetallic nanoparticles have higher adsorption affinity for lithium polysulfides and hold great potential in improving reaction kinetics. In this study, a nitrogen-doped carbon nanofiber carrier was prepared using high-voltage electrospinning technology, and through in-situ growth and high-temperature pyrolysis process, the carrier material was uniformly loaded with active sites of NiCo bimetallic nanoparticles derived from Metal-organic framework (MOF), aiming to improve the kinetics of sulfur oxidation and reduction and reduce the severe shuttle effect of soluble polysulfides. At the same time, polymethyl methacrylate was added to adjust the pore structure of the carbon nanofibers to form an ideal independent sulfur cathode porous conductive carbon network for rapid ion transport to prevent Li2S deposition and alleviate the volume change during lithiation/delithiation process. Experimental results show that the synergistic catalytic effect of bimetallic nanoparticles can not only rapidly anchor lithium polysulfides throughout the entire reaction process of Li-S batteries, but also reduce the resistance during the reaction process, accelerating the conversion of lithium polysulfides to Li2S deposition. It demonstrates outstanding electrochemical performance, with a first-cycle discharge specific capacity as high as 1431.7 mAh g−1 at a 0.2 C rate, and a Coulombic efficiency of 96%. After 500 cycles, its capacity still maintains at 628.5 mAh g−1, with a decay rate of only 0.11% per cycle. This study provides a feasible insight into the synergistic catalysis of MOF-derived metal nanoparticles, which has important guiding significance and potential impact on the catalysis of Li-S batteries by bimetallic nanoparticles with an independent sulfur cathode structure, and is expected to accelerate the industrialization process of Li-S batteries.