Enhanced Roles of Carbon Architectures in High-Performance Lithium-Ion Batteries

Highlights Assembly strategies that reinforce the roles of carbon architectures as active materials, electrochemical reaction frameworks, and current collectors in high-energy and high-power lithium-ion batteries are summarized. To enhance structural stability and volumetric performance, the rational design of carbon architectures for high-capacity noncarbons in terms of the interface, network skeleton, void space, and densification, is discussed in detail. Designing carbon cages that protect the electroactive noncarbon is highlighted as a promising strategy that solves the challenges associated with future high-capacity noncarbon anode construction. Lithium-ion batteries (LIBs), which are high-energy-density and low-safety-risk secondary batteries, are underpinned to the rise in electrochemical energy storage devices that satisfy the urgent demands of the global energy storage market. With the aim of achieving high energy density and fast-charging performance, the exploitation of simple and low-cost approaches for the production of high capacity, high density, high mass loading, and kinetically ion-accessible electrodes that maximize charge storage and transport in LIBs, is a critical need. Toward the construction of high-performance electrodes, carbons are promisingly used in the enhanced roles of active materials, electrochemical reaction frameworks for high-capacity noncarbons, and lightweight current collectors. Here, we review recent advances in the carbon engineering of electrodes for excellent electrochemical performance and structural stability, which is enabled by assembled carbon architectures that guarantee sufficient charge delivery and volume fluctuation buffering inside the electrode during cycling. Some specific feasible assembly methods, synergism between structural design components of carbon assemblies, and electrochemical performance enhancement are highlighted. The precise design of carbon cages by the assembly of graphene units is potentially useful for the controlled preparation of high-capacity carbon-caged noncarbon anodes with volumetric capacities over 2100 mAh cm −3 . Finally, insights are given on the prospects and challenges for designing carbon architectures for practical LIBs that simultaneously provide high energy densities (both gravimetric and volumetric) and high rate performance.