Automated Electroanalysis Accelerates the Discovery of Concerted Proton-Electron Transfer.

Area of Science:

• Electrochemistry
• Chemical Kinetics
• Materials Science

Background:

• Proton-coupled electron transfer (PCET) reactions are crucial for energy conversion and storage.
• Traditional electroanalysis of PCET reaction kinetics is labor-intensive, limiting research throughput.
• Manual experimentation hinders the exploration of complex reaction mechanisms.

Purpose of the Study:

• To develop and implement an automated, high-throughput electrochemical platform for PCET reaction analysis.
• To enhance the efficiency and speed of mechanistic inquiry in electrochemistry.
• To accelerate the discovery of novel reaction pathways and catalytic processes.

Main Methods:

• Development of an automated electrochemical system for high-throughput data acquisition.
• Utilized [Os^II(bpy)₂(py)(H₂O)]²⁺ as a model system for studying PCET kinetics.
• Analysis of over 43,800 voltammograms and quantification of approximately 730 kinetic rate constants.

Main Results:

• The automated platform increased research throughput by over 10-fold compared to manual methods.
• Identified a concerted PCET pathway involving adduct formation between the redox center and phosphate.
• Completed kinetic analysis in 66 days, a process that would take over 3 years manually.

Conclusions:

• Automated electroanalysis provides a powerful tool for rapid mechanistic investigation of PCET reactions.
• The generated 'big data' enables new research avenues previously inaccessible.
• This approach accelerates discoveries critical for advancing energy conversion and storage technologies.