Unlocking Mesoscopic Disorder in Graphitic Carbon with Spectroelectrochemistry

Area of Science:

• Materials Science
• Electrochemistry
• Spectroscopy

Background:

• Graphitic carbon electrodes are crucial for energy conversion and storage.
• Intrinsic defects in these electrodes can impact performance.
• Characterizing graphitic vs. disordered regions in bulk materials is challenging.

Purpose of the Study:

• To develop a method for differentiating graphitic regions from mesoscopic bulk disorder in carbon electrodes.
• To understand the influence of intrinsic defects on electrode properties under electrochemical conditions.

Main Methods:

• Utilized in-situ attenuated total reflectance infrared spectroscopy.
• Employed first-principles calculations.
• Applied electrochemical potential bias.

Main Results:

• Discovered electric-field dependent infrared activity in graphitic carbon electrodes.
• Showed this activity is sensitive to bulk mesoscopic intrinsic disorder.
• Identified opposing electric-field-dependent infrared responses between graphitic and amorphous domains.

Conclusions:

• The combined spectroscopic and computational approach allows for in-situ atomistic differentiation of graphitic and amorphous regions.
• This provides a roadmap for characterizing mesoscopic disorder in bulk carbon materials under potential bias.
• Enables better understanding and design of carbon electrodes for energy technologies.