Unraveling the Microstructure‐Property Relationship of Fe Single‐Atoms via Introducing Asymmetric P‐Coordination for Photocatalytic Hydrogen Evolution

Citations Over TimeTop 10% of 2024 papers

Abstract

Abstract The local atomic environments of single‐atom photocatalysts play a decisive role in determining the solar‐to‐hydrogen energy conversion efficiency. However, controllably modulating the microstructure of single‐atom sites to enhance catalytic activity and deeply understanding the structure‐property relationship remain great challenges. Herein, electron‐rich P atoms are introduced to accurately regulate the local coordination environment and electronic configuration of Fe single atoms and construct a unique asymmetrical FeN 3 P 2 motif into carbon nitride (FeN 3 P 2 ‐CN) for significantly improving the photocatalytic H 2 evolution activity and stability. Specifically, in the absence of noble metal cocatalyst and photosensitizer, the FeN 3 P 2 ‐CN achieves a remarkable H 2 evolution rate of 2668.5 µmol g −1 h −1 under visible light irradiation (λ > 420 nm), more than 105 times higher than that of unregulated FeN 4 sample. Systematic characterizations and theoretical calculations unveil that the FeN 3 P 2 single‐atom sites not only significantly broaden the photoabsorption region and facilitate the charge separation and interfacial transfer, but also efficiently promote adsorption and activation of H 2 O. This work paves a promising pathway to design novel single‐atom photocatalysts at the atomic level for achieving highly efficient water‐splitting performance.

Related Papers

• → Preparation, characterization and activity evaluation of p–n junction photocatalyst p-ZnO/n-TiO2(2008)271 cited
• → Photocatalysis: A novel approach to efficient demulsification(2015)29 cited
• The Assisted Excitations for Photocatalysis and Their Applications in Environment Treatments(2010)
• Underlayer Exposure Treatment of ZnO:Al-TiO_2 Coupled Film and Investigation to its Photocatalysis(2008)
• Preparation and photocatalytic activity of Fe~(3+)/Al~(3+)-TiO_2 composite photocatalyst and its the photocatalytic activity(2010)