"All in One" Strategy for Achieving Superprotonic Conductivity by Incorporating Strong Acids into a Robust Imidazole-Linked Covalent Organic Framework.

Luan, Tian-Xiang; Zhang, Pengtu; Wang, Qiurong; Xiao, Xin; Feng, Yijing; Yuan, Shiling; Li, Pei-Zhou; Xu, Qiang · Nano Lett · 2024

basic_science · Level V

Where this comes from

Abstract

The fabrication of solid-state proton-conducting electrolytes possessing both high performance and long-life reusability is significant but challenging. An "all-in-one" composite, <b>H</b><sub><b>3</b></sub><b>PO</b><sub><b>4</b></sub><b>@PyTFB-1-SO</b><sub><b>3</b></sub><b>H</b>, including imidazole, sulfonic acid, and phosphoric acid, which are essential for proton conduction, was successfully prepared by chemical post-modification and physical loading in the rationally pre-synthesized imidazole-based nanoporous covalent organic framework (COF), <b>PyTFB-1</b>. The resultant <b>H</b><sub><b>3</b></sub><b>PO</b><sub><b>4</b></sub><b>@PyTFB-1-SO</b><sub><b>3</b></sub><b>H</b> exhibits superhigh proton conductivity with its value even highly up to 1.15 × 10<sup>-1</sup> S cm<sup>-1</sup> at 353 K and 98% relative humidity (RH), making it one of the highest COF-based composites reported so far under the same conditions. Experimental studies and theoretical calculations further confirmed that the imidazole and sulfonic acid groups have strong interactions with the H<sub>3</sub>PO<sub>4</sub> molecules and the synergistic effect of these three groups dramatically improves the proton conductivity properties of <b>H</b><sub><b>3</b></sub><b>PO</b><sub><b>4</b></sub><b>@PyTFB-1-SO</b><sub><b>3</b></sub><b>H</b>. This work demonstrated that by aggregating multiple proton carriers into one composite, effective proton-conducting electrolyte can be feasibly achieved.