Dynamic single-site polysulfide immobilization in long-range disorder Cu-MOFs

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• The structural behavior of metal-organic frameworks (MOFs) during polysulfide electrode cycling is not well understood.
• Polysulfide electrolytes are crucial for advanced battery technologies, but their interaction with electrode materials needs clarification.

Purpose of the Study:

• To investigate the structural transformations of copper(II) 1,3,5-benzenetribonate (Cu3(BTC)2) metal-organic frameworks (MOFs) under electrochemical polysulfide conditions.
• To elucidate the mechanism of polysulfide interaction and immobilization within the MOF structure.

Main Methods:

• Electrochemical cycling of Cu3(BTC)2 MOFs in a polysulfide electrolyte.
• In-situ characterization techniques to observe structural changes during electrochemical processes.

Main Results:

• Demonstrated the electrochemical amorphization of Cu3(BTC)2 MOFs.
• Unveiled dynamic single-site polysulfide immobilization at interconvertible Cu2+/Cu+ centers.
• Observed reversible distortion of the Cu-O square planar units during polysulfide adsorption and desorption.

Conclusions:

• The study provides a detailed understanding of MOF structural dynamics in polysulfide environments.
• Findings offer insights into designing stable MOF-based electrodes for energy storage applications.