2D High-Entropy Phosphorus Chalcogenides for Efficient Solar-Driven CO₂ Reduction to Ethylene.

Area of Science:

• Materials Science
• Catalysis
• Renewable Energy

Background:

• Solar-driven CO2 reduction to ethylene (C2H4) is a promising energy storage method but faces thermodynamic challenges in CO2 activation and C-C coupling.
• High-entropy materials (HEMs), with multiple principal elements and high configurational entropy, are emerging as potential solutions for catalytic challenges.

Purpose of the Study:

• To develop a novel 2D high-entropy phosphorus chalcogenide (HEPC) photocatalyst for efficient solar-driven CO2 reduction to C2H4.
• To investigate the role of the multi-metal matrix and Cu active sites in enhancing CO2 activation and C-C coupling.

Main Methods:

• Rational design and synthesis of a 2D HEPC, Cu(CrVInFeMnNi)P2S6, by integrating multiple cations into a CuCrP2S6 framework.
• Characterization of the HEPC's structure and electronic properties.
• Evaluation of photocatalytic performance for CO2 to C2H4 conversion under visible light irradiation.

Main Results:

• The synthesized Cu(CrVInFeMnNi)P2S6 exhibited excellent photocatalytic activity for CO2 reduction to C2H4, achieving an ultrahigh apparent quantum yield (AQY) of 7.4% at 475 nm.
• High selectivity for C2H4 (71%) was achieved under sacrificial-agent-free conditions.
• The Cu site was identified as the dominant active center, supported by the multi-metal matrix that enhances electron donation and C-C coupling.

Conclusions:

• The developed HEPC, Cu(CrVInFeMnNi)P2S6, demonstrates superior performance in solar-driven CO2 to C2H4 conversion, outperforming existing state-of-the-art photocatalysts.
• This work pioneers the application of high-entropy phosphorus chalcogenides in catalysis, offering a new strategy for designing efficient multifunctional photocatalysts.
• The findings provide valuable insights into utilizing HEMs for sustainable energy solutions and chemical synthesis.