Converting a metal-coordinating polymer to a polymerized ionic liquid improves Li+ transport

Solid polymer electrolytes (SPEs) with mechanical strength and reduced flammability may also enable next-generation Li+ batteries with higher energy densities. However, conventional SPEs have fundamental limitations in terms of Li+ conductivity. While an imidazole functionalized polymer (PMS-Im) has been previously shown to have ionic conductivity related to the imidazole-Li+ coordination, herein we demonstrate that quaternization of this polymer to form an analogous imidazolium functionalized polymer (PMS-Im+) more efficiently solvates lithium salts and plasticizes the polymer. In addition, inverse Haven ratios as high as 10 indicate positively correlated Li+ transport, possibly due to percolation of nanochannels that significantly improve battery-relevant conductivity. From these combined effects, Li+ conductivity in PMS-Im+ (2.1*10-5 S/cm) is over an order of magnitude greater than in PMS-Im at 90 °C (1.6*10-6 S/cm)., See supporting information from published main text. https://doi.org/10.1021/acsmacrolett.4c00704 In short, polymers were synthesized via anionic polymerization and subsequently functionalized through multiple steps. Polymers were then blended with Li salts and characterized via thermal, electrochemical, and spectroscopic methods., , # Converting a metal-coordinating polymer to a polymerized ionic liquid improves Li+ transport

[https://doi.org/10.5061/dryad.m37pvmdcg](https://doi.org/10.5061/dryad.m37pvmdcg)

## Description of the data and file structure

See supporting information from published main text. [https://doi.org/10.1021/acsmacrolett.4c00704](https://doi.org/10.1021/acsmacrolett.4c00704) In short, polymers were synthesized via anionic polymerization and subsequently functionalized through multiple steps. Polymers were then blended with Li salts and characterized via thermal, electrochemical, and spectroscopic methods.

### Files and variables

#### File: RawData.zip

**Description:** Files are organized into folders based on figure number from the corresponding manuscript: A. B. C... = folder names, a. b. c... = file names within folder, 1. 2. 3... = column names within file. The file list is followed by a list of variable names and descriptions.

A. Figure 2

```
a. Figure 2a.csv

1\. PMS-Im r03 ...