Aqueous electrochromic battery (ECB) is a multifunctional
technology
that shows great potential in various applications including energy-saving
buildings and wearable batteries with visible energy levels. However,
owing to the mismatch between traditional electrochromic materials
and the electrolyte, aqueous ECBs generally exhibit poor cycling stability
which bottlenecks their practical commercialization. Herein, we present
an ultrastable electrochromic system composed of lithium titanate
(Li4Ti5O12, LTO) electrode and Al3+/Zn2+ hybrid electrolyte. The fully compatible
system exhibits excellent redox reaction reversibility, thus leading
to extremely high cycling stabilities in optical contrast (12 500
cycles with unnoticeable degradation) and energy storage (4000 cycles
with 82.6% retention of capacity), superior electrochromic performances
including high optical contrast (∼74.73%) and fast responses
(4.35 s/7.65 s for bleaching/coloring), as well as excellent discharge
areal capacity of 151.94 mAh m–2. The extraordinary
cycling stability can be attributed to the robust [TiO6] octahedral frameworks which remain chemically active even upon
the gradual substitution of Li+ with Al3+ in
LTO over multiple operation cycles. The high-performance electrochromic
system demonstrated here not only makes the commercialization of low-cost,
high-safety aqueous-based electrochromic devices possible but also
provides potential design guidance for LTO-related materials used
in aqueous-based energy storage devices.