Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges

Electrolyte additives have been explored to attain significant breakthroughs in the long-term cycling performance of lithium-ion batteries (LIBs) without sacrificing energy density; this has been achieved through the development of stable electrode interfacial structures and the elimination of reactive substances. Here we highlight the potential and the challenges raised by studies on electrolyte additives toward addressing the interfacially induced deterioration of high-capacity electrodes with a focus on Ni-rich layered oxides and Si, which are expected to satisfy the growing demands for high-energy-density batteries. We also discuss issues with the design of electrolyte additives for practical viability. A deep understanding of the roles of existing electrolyte additives depending on their functional groups will aid in the design of functional additive moieties capable of building robust interfacial layers, scavenging undesired reactive species, and suppressing the gas generation that causes safety hazards and shortened lifetimes of LIBs.