Electrochemiluminescence Illuminates Single-Atom Catalysts: Real-Time Atomic-Scale Dynamics and Operando Electronic...

Area of Science:

• Catalysis
• Materials Science
• Spectroscopy

Background:

• Single-atom catalysts (SACs) offer precisely defined active sites for electrocatalysis.
• Characterizing SACs under working conditions is challenging due to limitations of static or ensemble-averaged techniques.

Purpose of the Study:

• To review electrochemiluminescence (ECL) as an operando probe for single-atom catalysis.
• To establish a framework linking SAC structure, intermediate chemistry, and ECL emission.
• To highlight ECL's potential for quantitative structural analysis of SACs.

Main Methods:

• Discussion of ECL as a structure-informative probe, not just signal amplification.
• Analysis of signal-conversion framework relating active-site structure to photon emission.
• Emphasis on advanced ECL techniques: potential-resolved, time-dependent, super-resolution microscopy, and multimodal analysis.

Main Results:

• ECL can reveal active-site identity, density, coordination, electronic/spin structure, intermediates, and heterogeneity.
• Recent advances enable detailed, dynamic insights into SACs during catalysis.
• ECL bridges the gap between static atomic structure and dynamic catalytic function.

Conclusions:

• ECL is a promising technique for operando structural characterization of SACs.
• Further development is needed to transition ECL from a qualitative reporter to a quantitative tool.
• ECL facilitates a deeper mechanistic understanding of single-atom catalysis.