Integrating electronic structure regulation and dynamic active sites construction on Ni_xCd_1-xS-Ni⁰ photocatalyst for...

Area of Science:

• Materials Science
• Photocatalysis
• Renewable Energy

Background:

• Optimizing photocatalyst electronic structure and active sites is crucial for efficient hydrogen evolution.
• Nickel-doped cadmium sulfide (Ni_xCd_1-xS) offers potential for photocatalytic applications.
• Developing sustainable and dynamic active sites is key to improving reaction kinetics.

Purpose of the Study:

• To synthesize a novel Ni_xCd_1-xS-Ni⁰ photocatalyst with surface Ni doping and atomic Ni⁰ anchoring sites.
• To investigate the role of Ni doping in modulating the electronic structure for enhanced sulfur atom activity.
• To explore the function of photogenerated Ni⁰ as charge transfer bridges and dynamic active sites for hydrogen production.

Main Methods:

• Synthesis of Ni_xCd_1-xS-Ni⁰ via Ni²⁺ ion exchange and in-situ photo-induction of Ni⁰.
• Characterization of electronic structure modifications due to Ni doping and Ni⁰ anchoring.
• Evaluation of photocatalytic hydrogen evolution activity and quantum efficiency under visible light irradiation.

Main Results:

• Ni doping introduces hybridized states, optimizing the electronic structure of sulfur atoms.
• Photogenerated Ni⁰ atoms act as bridges, facilitating the reduction of Ni²⁺ to Ni clusters.
• The Ni_xCd_1-xS-Ni⁰ photocatalyst achieved a high hydrogen evolution rate (428 mmol·h^-1·g^-1) and quantum efficiency (75.6% at 420 nm).

Conclusions:

• The developed Ni_xCd_1-xS-Ni⁰ photocatalyst demonstrates an optimal sulfur electronic structure for photocatalytic H₂ evolution.
• Dynamic Ni clusters formed via photo-deposition/dissolution provide sustainable reaction centers and enhance redox kinetics.
• This dual pathway approach, combining electronic structure modulation and dynamic active sites, opens new avenues for efficient water reduction.