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Operando Spectroscopy Observation of Mo Clusters-Ti3 C2 TX Catalyst/Support Interface's Dynamic Evolution in Hydrogen
Peng Fei Wu1, Yu Qi Yang2, Hong Yan Xi1
1Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing, 100191, China.
Nitrogen-doped molybdenum atom-clusters on Ti3C2Tx transform into highly active monatomic structures during hydrogen evolution reactions (HER), boosting catalytic performance. This dynamic evolution reveals key insights into catalyst behavior and interfacial mechanisms.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Catalyst-support interactions are crucial for electrocatalytic hydrogen evolution (HER) performance, often influenced by phase transitions or structural changes.
- Understanding the dynamic evolution of catalyst interfaces, structural transformations, and stability under working conditions remains challenging.
- Operando techniques are essential for real-time monitoring of dynamic changes and identification of active sites during reactions.
Purpose of the Study:
- To investigate the dynamic evolution of nitrogen-doped molybdenum atom-clusters on Ti3C2Tx (MoACs/N-Ti3C2Tx) during the hydrogen evolution reaction (HER).
- To reveal the intrinsic behavior, interfacial dynamics, and structural transformations of the model catalyst under electrochemical bias.
- To correlate structural evolution with catalytic performance and identify the active species responsible for enhanced HER.
Main Methods:
- Utilized a model catalyst: nitrogen-doped molybdenum atom-clusters on Ti3C2Tx (MoACs/N-Ti3C2Tx).
- Employed operando X-ray absorption structure (XAS) and in situ Raman spectroscopy to monitor structural changes in real-time.
- Performed theoretical calculations to support experimental observations and understand reaction mechanisms.
Main Results:
- Observed the dynamic evolution of Mo clusters into a 6-coordinated monatomic Mo structure under HER working conditions.
- Demonstrated that this structural transformation exposes more active sites, significantly enhancing catalytic performance.
- Achieved excellent HER performance comparable to commercial Pt/C, with a low overpotential (60 mV at 10 mA cm-2) and Tafel slope (56 mV dec-1).
Conclusions:
- The dynamic structural evolution of Mo clusters to monatomic Mo species is key to the enhanced HER activity of MoACs/N-Ti3C2Tx.
- This study provides critical insights into interfacial migration mechanisms and the origin of activity enhancement in electrocatalysts.
- The findings offer a new perspective for designing and understanding advanced electrocatalytic materials for energy conversion.
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