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Catalysis02:50

Catalysis

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The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
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Reduction of Alkenes: Catalytic Hydrogenation02:13

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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

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Small (Weinheim an Der Bergstrasse, Germany)
|October 20, 2023
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Summary

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.

Keywords:
Ti3C2TXhydrogen evolution reactionin situ Raman spectroscopymo clustersoperando X-ray absorption structure (XAS)

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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.