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Topotactic Nitridation Enabled Core-Shell La4Ti3(O,N)12@LaTiO2N for Efficient Photoelectrochemical Water Splitting
Jeongsuk Seo1, Yoonji Seo1, Ohmin Kwon2
1Department of Chemistry, College of Natural Sciences, Chonnam National University, Gwangju, South Korea.
Layered perovskite oxynitrides show promise for water splitting. This study reveals a gradual nitridation mechanism, enabling core-shell heterostructures with enhanced photoelectrochemical activity.
Area of Science:
- Materials Science
- Photocatalysis
- Inorganic Chemistry
Background:
- Layered perovskite oxynitrides are promising semiconductors for photocatalytic water splitting due to their electronic and structural properties.
- Challenges in synthesis, including structural collapse during nitridation, hinder the development of efficient materials and obscure reaction mechanisms.
Purpose of the Study:
- To systematically investigate the nitridation mechanism of layered perovskites.
- To understand how nitridation influences the formation of heterostructures for enhanced photocatalysis.
- To provide insights into the synthesis of efficient perovskite oxynitrides for solar water splitting.
Main Methods:
- Neutron diffraction and electron microscopy were employed to study the nitridation process.
- Systematic investigation of the nitridation of La4Ti3O12.
- Fabrication and characterization of core-shell heterostructures (La4Ti3(O,N)12@LaTiO2N).
Main Results:
- Nitridation proceeds topotactically, gradually and heterogeneously, preserving the layered framework.
- N-substituted layered perovskite oxynitride forms before complete conversion to 3D perovskite.
- A layered/3D core-shell heterostructure (La4Ti3(O,N)12@LaTiO2N) was successfully synthesized.
- The core-shell structure exhibits improved charge carrier dynamics and enhanced photoelectrochemical water splitting activity.
Conclusions:
- Layered oxynitrides are crucial for heterojunction formation and band alignment in photocatalysts.
- The study elucidates the nitridation mechanism of layered perovskites, revealing a pathway for creating core-shell structures.
- The synthesized core-shell photoanode demonstrates significantly improved water splitting performance, offering a viable route for efficient perovskite oxynitrides.
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