High-entropy sulfides (HESs) have emerged as a groundbreaking class of materials for photocatalysis due to their unique compositional complexity and tunable electronic properties. Recent studies have demonstrated that HESs, such as (FeCoNiCuZn)S, exhibit exceptional light absorption across a broad spectrum, with bandgaps ranging from 1.2 to 2.5 eV, enabling efficient utilization of solar energy. For instance, (FeCoNiCuZn)S achieved a hydrogen evolution rate of 12.8 mmol g⁻¹ h⁻¹ under visible light irradiation, surpassing traditional binary sulfides like CdS (3.2 mmol g⁻¹ h⁻¹) by a factor of four. This enhanced performance is attributed to the synergistic effects of multiple metal cations, which optimize charge carrier dynamics and reduce recombination rates.
The high configurational entropy in HESs stabilizes the crystal structure and introduces lattice distortions, leading to improved photocatalytic stability and durability. A study on (CrMnFeCoNi)S revealed that the material retained 95% of its initial activity after 100 hours of continuous operation, compared to only 60% for MoS₂ under identical conditions. The lattice strain induced by the random distribution of metal cations also facilitates the formation of active sites, as evidenced by a 3-fold increase in surface area (up to 150 m² g⁻¹) compared to conventional sulfides. These structural advantages make HESs highly resistant to photocorrosion, a common issue in sulfide-based photocatalysts.
The electronic structure engineering in HESs enables precise control over redox potentials, making them versatile for diverse photocatalytic applications. For example, (TiVNbMoW)S demonstrated a CO₂ reduction efficiency of 8.7 μmol g⁻¹ h⁻¹ with a selectivity of 92% toward CH₄, outperforming traditional catalysts like TiO₂ (1.2 μmol g⁻¹ h⁻¹). The multi-element composition allows for fine-tuning of the conduction and valence band positions, optimizing the thermodynamic driving force for specific reactions. Density functional theory (DFT) calculations further confirmed that the d-band center modulation in HESs enhances adsorption energies for key intermediates, improving overall catalytic efficiency.
Scalability and cost-effectiveness are critical factors for the practical deployment of HES-based photocatalysts. Recent advancements in solution-phase synthesis have enabled large-scale production of HES nanoparticles with yields exceeding 90%. A pilot-scale study using (FeCoNiCuZn)S achieved a production cost of $15 per gram, significantly lower than noble metal-based catalysts like Pt/TiO₂ ($50 per gram). Additionally, the use of earth-abundant elements in HESs aligns with sustainability goals, reducing reliance on scarce resources while maintaining high performance.
Future research directions for HESs in photocatalysis include exploring their potential in tandem systems and integrating them with other functional materials such as graphene or perovskites. Preliminary results from a hybrid system combining (FeCoNiCuZn)S with graphene oxide showed a remarkable hydrogen evolution rate of 18.4 mmol g⁻¹ h⁻¹ under simulated sunlight, highlighting the potential for synergistic effects. Furthermore, computational screening methods are being developed to identify optimal compositions and predict performance metrics, accelerating the discovery of next-generation HES photocatalysts.
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