Layered High‐Entropy Metallic Glasses for Photothermal CO₂ Methanation

Abstract High entropy alloys and metallic glasses, as two typical metastable nanomaterials, have attracted tremendous interest in energy conversion catalysis due to their high reactivity in nonequilibrium states. Herein, a novel nanomaterial, layered high entropy metallic glass (HEMG), in a higher energy state than low‐entropy alloys and its crystalline counterpart due to both the disordered elemental and structural arrangements, is synthesized. Specifically, the MnNiZrRuCe HEMG exhibits highly enhanced photothermal catalytic activity and long‐term stability. An unprecedented CO₂ methanation rate of 489 mmol g⁻¹ h⁻¹ at 330 °C is achieved, which is, to the authors’ knowledge, the highest photothermal CO₂ methanation rate in flow reactors. The remarkable activity originates from the abundant free volume and high internal energy state of HEMG, which lead to the extraordinary heterolytic H₂ dissociation capacity. The high‐entropy effect also ensures the excellent stability of HEMG for up to 450 h. This work not only provides a new perspective on the catalytic mechanism of HEMG, but also sheds light on the great catalytic potential in future carbon‐negative industry.