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Photo- and electrocatalytic conversion driven by transition metal-assisted ferroelectric heterojunction.

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Ferroelectric polarization switching in TM@g-ZnO/In2Se3 heterostructures enhances catalytic activity for hydrogen evolution and oxygen reactions. This enables tunable photo- and electrocatalysis, driven by electronic phase transitions.

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Density functional theoryFerroelectric heterojunctionsHydrogen evolution reactionOxygen evolution and reduction reactionPhoto- and electrocatalytic conversion

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Area of Science:

  • Materials Science
  • Catalysis
  • Computational Chemistry

Background:

  • Ferroelectric polarization switching offers dynamic control over material properties.
  • Electronic phase transitions are key to modulating catalytic activity.
  • Heterostructures of transition metal-doped graphene-zinc oxide (TM@g-ZnO) and indium selenide (In2Se3) are promising catalytic platforms.

Purpose of the Study:

  • To investigate the catalytic activities (HER, OER, ORR) of TM@g-ZnO/In2Se3 heterostructures.
  • To explore the mechanism of polarization-induced semiconductor-to-metal transitions for photo- and electrocatalysis.
  • To identify factors governing catalytic performance using machine learning.

Main Methods:

  • Density functional theory (DFT) calculations.
  • Non-adiabatic molecular dynamics simulations.
  • Machine learning analysis.

Main Results:

  • Pt@g-ZnO/In2Se3 shows excellent hydrogen evolution reaction (HER) performance.
  • Ni@g-ZnO/↓-In2Se3 and Pd@g-ZnO/↑-In2Se3 exhibit bifunctional oxygen evolution (OER) and reduction (ORR) activities.
  • Polarization enables semiconductor-to-metal transitions, facilitating interconversion between photocatalysis and electrocatalysis.
  • TM@g-ZnO/↑-In2Se3 demonstrates long hot-carrier lifetime for photocatalysis, while TM@g-ZnO/↓-In2Se3 shows high electrical conductivity for electrocatalysis.

Conclusions:

  • TM@g-ZnO/In2Se3 heterostructures are efficient multifunctional catalysts.
  • Polarization-induced phase transitions are crucial for tunable photoelectrocatalytic performance.
  • The d-electron number of transition metal dopants is a primary determinant of catalytic activity.