Dynamic Solvation Structure Regulation Enables Long-Life Li–Organic Batteries

Li–organic batteries with organic carbonyl electrode materials (OCEMs) have been considered as a sustainable energy storage technology, while suffering from a critical challenge regarding the high dissolution of OCEMs in electrolytes. To address this problem, conventional strategies primarily focus on modulating static solvent–OCEM interactions but often overlook the role of dynamic solvation structure in governing the dissolution behavior of OCEMs. Here, we propose a dynamic solvation structure regulation strategy to address the degradation of OCEMs during dynamic electrochemical processes and thus achieve long-life Li–organic batteries. In traditional electrolytes, the OCEMs could displace anions to participate in solvation during dynamic electrochemical processes, thereby exacerbating the continuous dissolution of OCEMs. A series of solvation structure stabilizers were thus screened to address the dynamic solvation structure disruption issue. Among them, 2 H,3 H -decafluoropentane (DFP) exhibits the weakest interaction with OCEMs while maintaining moderate interactions with key electrolyte components, thereby reinforcing the stability of the solvation structure and effectively isolating OCEMs from the solvation network during dynamic electrochemical processes. The optimal solvation-isolating electrolyte (SIE) enables Li–pyrene-4,5,9,10-tetraone (Li–PTO) batteries to deliver exceptional cycling stability, retaining 67% of its capacity after 1400 cycles at 2 C, along with a high-rate capacity of 236.7 mAh g –1 at 5 C. This study shifts the design paradigm from static dissolution suppression to dynamic solvation-structure stabilization, providing a generalizable electrolyte-engineering principle for achieving long-life Li–organic batteries.