LiFePO4 quantum-dots composite synthesized by a general microreactor strategy for ultra-high-rate lithium ion batteries

Abstract

Due to the relatively slow, diffusion-controlled faradaic reaction mechanisms of conventional LiFePO4 (LFP) materials, which is hard to deliver satisfied capacity for high rate applications. In this work, ultrafine LFP quantum dots (LFP-QDs) co-modified by two types of carbonaceous materials - amorphous carbon and graphitized conductive carbon (graphene) have been successfully synthesized through a novel microreactor strategy. Because of the very limited area constructed by the dual-carbon microreactor for the growth of LFP crystal, it's demension was furthest suppressed to a very small level (~ 6.5nm). Such a designed nano-composite possesses a large specific surface area for charge adsorption and abundant active sites for faradaic reactions, as well as ideal kinetic features for both electron and ion transport, and thus exhibits ultra-fast, surface-reaction-controlled lithium storage behavior, mimicking the pseudocapacitive mechanisms for supercapacitor materials, in terms of extraordinary rate capability (78mAhg−1 at 200C) and remarkable cycling stability (~ 99% over 1000 cycles at 20C). On the other side, due to the quasi-2D structure of the synthesized LFP-QDs composite, which can be used as the basic unit to further fabricate free-standing film, aerogel and fiber electrode without the addition of binder and conductive agent for different practical applications. In addition, to deeper understand its electrochemical behavior, a combined experimental and density functional theoretical (DFT) calculation study is also introduced.