Lattice-Embedded Single-Atom Sr-O-Ni Channels Enable Photon-Phonon Coupling for Photothermal N2O Decomposition

Area of Science:

• Materials Science
• Catalysis
• Environmental Science

Background:

• Nitrous oxide (N₂O) is a potent greenhouse gas with challenging industrial abatement.
• Current thermocatalytic and photocatalytic methods for N₂O decomposition have limitations in energy input or efficiency.
• Synchronizing thermal and catalytic processes at the atomic scale is crucial for enhanced performance.

Purpose of the Study:

• To develop a novel photothermal catalytic system for efficient N₂O decomposition.
• To investigate the role of lattice-embedded single atoms in synchronizing charge and heat transfer.
• To achieve high N₂O conversion under solar irradiation without external heating.

Main Methods:

• Synthesis of a lattice-embedded single-atom catalyst by incorporating Sr into NiO.
• Characterization using techniques like X-ray diffraction and spectroscopy.
• Testing N₂O decomposition efficiency under simulated and outdoor sunlight.
• Computational analysis using Density Functional Theory (DFT) and operando spectroscopy.

Main Results:

• Sr-embedded NiO (Sr₁-NiO) achieved 97.2% single-pass conversion of 10 vol % N₂O under simulated sunlight.
• The catalyst demonstrated a high conversion rate of 43.2 mmol g⁻¹ h⁻¹.
• Stable operation exceeding 200 hours was observed, with robustness against O₂, NO, and H₂O.
• Mechanism elucidated through DFT and spectroscopy, highlighting Sr-O-Ni channels for charge and phonon transfer.

Conclusions:

• Lattice-embedded single-atom channels provide an effective strategy for synchronizing photothermal catalysis.
• The developed Sr₁-NiO catalyst offers a highly efficient and stable solution for N₂O abatement.
• This approach represents a general chemical motif for advancing photothermal catalysis for environmental applications.