High-Capacity NH4+ Charge Storage in Covalent Organic Frameworks

Zhengnan Tian; Vinayak S Kale; Yizhou Wang; Sharath Kandambeth; Justyna Czaban-Jóźwiak; Osama Shekhah; Mohamed Eddaoudi; Husam N Alshareef

doi:10.1021/jacs.1c09290

High-Capacity NH₄⁺ Charge Storage in Covalent Organic Frameworks

J Am Chem Soc. 2021 Nov 17;143(45):19178-19186. doi: 10.1021/jacs.1c09290. Epub 2021 Nov 5.

Authors

Zhengnan Tian¹, Vinayak S Kale², Yizhou Wang¹, Sharath Kandambeth², Justyna Czaban-Jóźwiak², Osama Shekhah², Mohamed Eddaoudi², Husam N Alshareef¹

Affiliations

¹ Materials Science and Engineering, Physical Science and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.
² Advanced Membranes and Porous Materials Center, Physical Science and Engineering Division, Functional Materials Design, Discovery and Development Research Group (FMD3), King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.

PMID: 34739750
DOI: 10.1021/jacs.1c09290

Abstract

Ammonium ions (NH₄⁺), as non-metallic charge carriers, have spurred great research interest in the realm of aqueous batteries. Unfortunately, most inorganic host materials used in these batteries are still limited by the sluggish diffusion kinetics. Here, we report a unique hydrogen bond chemistry to employ covalent organic frameworks (COFs) for NH₄⁺ ion storage, which achieves a high capacity of 220.4 mAh g^-1 at a current density of 0.5 A g^-1. Combining the theoretical simulation and materials analysis, a universal mechanism for the reaction of nitrogen and oxygen bridged by hydrogen bonds is revealed. In addition, we explain the solvation behavior of NH₄⁺, leading to a relationship between redox potential and desolvation energy barrier. This work provides a new insight into NH₄⁺ ion storage in host materials based on hydrogen bond chemistry. This mechanism can be leveraged to design and develop COFs for electrochemical energy storage.