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ATR-SEIRAS for Single-Atom Electrocatalysis.

Yinyin Wang1, Jie Ding2, Chenliang Su1

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Single-atom catalysts (SACs) are advanced materials for energy technologies. Attenuated total reflection-surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals their reaction mechanisms and stability, aiding the design of efficient catalysts.

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Area of Science:

  • Heterogeneous catalysis and electrochemistry.
  • Materials science and nanotechnology.
  • Spectroscopic characterization techniques.

Background:

  • Single-atom catalysts (SACs) offer high atom efficiency and well-defined active sites for catalysis.
  • Electrochemical energy conversion and storage technologies benefit from SACs' unique properties.
  • Mechanistic elucidation of complex proton-coupled electron transfer processes in SACs remains challenging.

Purpose of the Study:

  • To demonstrate the application of attenuated total reflection-surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) for characterizing single-atom electrocatalysts.
  • To elucidate structure-activity relationships of SACs in CO/CO2 reduction reaction (CO/CO2RR), oxygen reduction reaction (ORR), and nitrate reduction reaction (NO3-RR).
  • To highlight the role of ATR-SEIRAS in understanding SACs' stability, active site function, and dynamic structural evolution.

Main Methods:

  • Utilized ATR-SEIRAS for *in situ/operando* characterization of single-atom electrocatalysts.
  • Analyzed ATR-SEIRAS enhancement mechanisms (physical and chemical).
  • Identified vibrational fingerprints of reaction intermediates (oxygen-containing, carbonaceous, nitrogenous) and adsorbates.

Main Results:

  • ATR-SEIRAS effectively traced reaction pathways in SACs by identifying key intermediates.
  • Demonstrated ATR-SEIRAS's capability in studying the stability and active site function of SACs during CO/CO2RR, ORR, and NO3-RR.
  • Validated density functional theory (DFT) calculations using ATR-SEIRAS data for SACs.

Conclusions:

  • ATR-SEIRAS is a powerful tool for mechanistic studies of single-atom electrocatalysis.
  • Understanding active site dynamics and reaction mechanisms through ATR-SEIRAS aids in designing high-performance, durable SACs.
  • This work provides insights for advancing electrochemical energy conversion and storage technologies using SACs.