Composite solid-state electrolytes with fast ion channels constructed from in-situ hydrogen bonding and coupling/crosslinking effects for dendrite-free solid-state lithium batteries

All-solid-state lithium battery (ALLSB) with organic/inorganic composite solid-state electrolyte (CSSE) is one of the candidates for future energy storage due to the high specific energy and safety. However, large impedances and incompatibilities at the rigid electrode/electrolyte and internal interfaces of CSSE remain stumbling blocks for the spread of ASSLB. Acrylamide (AM)-contained (3-methacrylamidopropyl) triethoxysilane (MTS) is incorporated into CSSE to optimize the interfaces and modulate the ion diffusion and deposition behaviors based on the in-situ synergy effects of coupling/crosslinking and hydrogen bonding. Multiple hydrogen bonds between CSSEs and polar AM groups construct diverse Li interactions and facilitate dissociation and diffusion of Li. Coupling/crosslinking effect of the MTS can in-situ rearrange the above diversified Li environment. In turn, hydrogen bonds strengthen the coupling effect to the interface. The synergistic function contributes to favorable interfacial compatibility and stability, establishing a fast ion transport channel in the ASSLB. The MTS-intervened CSSE exhibits superior electrochemical and thermal properties. Li symmetric cells with this functional CSSE demonstrate stable lithium deposition/extraction for up to 2000 h. Moreover, the Li|LiFePO4 battery retains 91.7 % of its capacity after 500 cycles. This in-situ synergistic regulation provides a rational and simple guide for enhancing interface stability in CSSE and ASSLB.