Abstract：Carbon solely can form a lot of nanostructures, such as zero-dimensional nanosphere, one-dimensional nanotube and two-dimensional graphene. They perform differently in Li-ion and Li-S batteries. It is worth noting that CNTs and graphene are not appropriate to be used as electroactive materials for Li-ion or Li-S batteries for four reasons. First, when CNTs and graphene are used as an anode, they often exhibit high specific capacities during the first lithiation step, but a large fraction of lithium ions is irreversibly consumed instead of reversibly stored, leading to a low Coulombic efficiency of the cell. Second, a graphene-based anode has a large voltage hysteresis in the charge/discharge curves. Third, it has been reported a CNT-based anode lacks a steady voltage plateau with large change in voltage during discharge. Fourth, despite their high initial capacities, graphene and CNT-based anodes often suffer from fast capacity decay after a few tens of cycles. Continuous efforts have been made to build better lithium batteries with a higher energy density and wider applicability, including both current state-of-the-art Li-ion batteries and near-term Li-S batteries. Because the behavior of a rechargeable battery is mainly based on the performance of its anode and cathode, designing advanced electrode materials as well as electrode with tailored compositions and structures has been the hot topic in recent years. The role of carbon nano-materials to construct electrode materials and tailored electrodes in Li-ion and Li-S batteries in high performance was reviewed in the paper from three aspects. Firstly, the role of carbon nano-materials in modifying the electroactive materials was discussed from three aspects:electron- and ion-transport facilitators, immobilization sites and volume expansion buffering. Secondly, the role of carbon nano-materials in optimizing the inactive components was considered as follows:conducting additives, current collectors and conductive interlayers. Thirdly, the role of carbon nano-materials in designing the bendable and stretchable devices are discussed from three aspects:conductive phases in nonconductive substrates, flexible current collectors and freestanding composite electrode. Finally, perspectives on future development of Li-ion and Li-S batteries were presented. It is considered that multi-functional carbon nano-materials will be main research focus in the future.
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