High-entropy-alloy nanoparticles (HEA-NPs) composed of 3d transition metallic elements have attracted intensive attention in photothermal conversion regions due to their d-d interband transitions (IBTs). However, the effect arising from the unbalanced elemental ratio still needs more focus. In this work, FeCoNiCrMn HEA-NPs with different elemental ratios among Cr and Mn have been employed to clarify the impact of different composed elements on the optical absorption and photothermal conversion performance. It can be recognized that the unbalanced elemental ratio of HEA-NPs can reduce the photothermal performance. Density functional theory calculation demonstrated that d-d IBTs can be changed by the different composed element ratios, resulting in a number of insufficient filling regions around the Fermi level (±4 eV). As a result, the HEA-NPs (FeCoNiCrMn) with a balanced elemental ratio exhibit the highest surface temperature of 97.6 °C under 1 sun irradiation, and the evaporation rate and energy conversion efficiency could reach 2.13 kg·m·h and 93%, respectively, demonstrating effective solar steam generation behavior.
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