Electrolytes
have played critical roles in electrochemical energy
storage. In Li-ion battery, liquid electrolytes have shown their excellent
performances over decades, such as high ionic conductivity (∼10–3 S cm–1) and good contacts with
electrodes. However, the use of liquid electrolytes often brought
risks associated with leakage and combustion of organic electrolytes.
Hence, polymer electrolytes become potential candidates to replace
liquid electrolyte systems. Although solid polymer electrolytes (SPEs)
offer better safety and good mechanical properties to take over liquid
electrolytes, most of them only deliver low ionic conductivities (∼10–8 S cm–1) and poor contact with electrodes,
resulting in poor cycle performance and low electrical capacity of
the batteries. In addition, gel polymer electrolytes (GPEs) have received
increasing research attention due to their relevant characteristics,
which extend from liquid electrolytes and solid polymer electrolytes.
In this review, state-of-the-art samples of gel polymer electrolytes
are elucidated with respect to their structural design and electrochemical
properties to determine their application potential in Li-ion batteries
(LIBs). First, we present the general requirements of GPEs for LIBs
applications, followed by important electrochemical properties of
GPEs for LIBs including ionic conductivity, transference number, and
ionic transport mechanisms. Furthermore, recent progress of common
polymers, namely, polyether, polyvinyl, polynitrile, polycarbonate,
and polyacrylate, as polymer host of GPEs has been carefully explained.
Finally, the alternative polymers were also discussed to provide new
approaches for further developments of GPEs to fulfill the demanded
properties for practical applications.