An ultralow-charge-overpotential and long-cycle-life solid-state Li-CO2 battery enabled by plasmon-enhanced solar photothermal catalysis

Lithium-carbon dioxide (Li-CO 2 ) batteries , especially solid-state Li-CO 2 batteries , have attracted much attention due to the high energy density and potential application of carbon neutrality. However, the extremely sluggish kinetics of CO 2 evolution reaction in the batteries result in a notorious high-charge-potential over 4.0 V, thus impeding the development of Li-CO 2 batteries. Here, by in-situ constructing a plasmonic Ru/Li 2 CO 3 -based heterostructure , we report an ultra-low charge overpotential and long cycle life solid-state Li-CO 2 battery via the energetic hot carries produced by nonradiative decay of localized surface plasmons where solar energy can be efficintly harvested (over 90% absorption efficiency from 200 nm to 1000 nm), concentrated and converted on the plasmonic Ru catalysts. Experimental results show that the plasmonic photothermal catalysis using Ru catalysts can catalyze C-O bond cleavage and construct a plasmonic Ru/Li 2 CO 3 -based heterostructure in the battery on discharge, and effectively accelerate the CO 2 envolution reaction via injecting the hot carriers generated from the plasmonic Ru catalysts into the discharged Li 2 CO 3 -based products on charge. As a result, by using a chemically stable and high Li-ion conductive MSI layer , the battery shows a record low charge potential (2.99 V) even after a long-term cycling (over 450 cycles) operating at 500 mA g −1 at 500 mAh g −1 . This battery technology paves the way for developing next-generation high-specific-energy Li-CO 2 batteries with carbon neutrality.