Cu-based nanocatalysts are the cornerstone of various industrial catalytic processes. Synergistically strengthening the catalytic stability and activity of Cu-based nanocatalysts is an ongoing challenge. Herein, the high-entropy principle is applied to modify the structure of Cu-based nanocatalysts, and a PVP templated method is invented for generally synthesizing six-eleven dissimilar elements as high-entropy two-dimensional (2D) materials. Taking 2D Cu₂Zn₁Al_0.5Ce₅Zr_0.5O_x as an example, the high-entropy structure not only enhances the sintering resistance from 400 °C to 800 °C but also improves its CO₂ hydrogenation activity to a pure CO production rate of 417.2 mmol g⁻¹ h⁻¹ at 500 °C, 4 times higher than that of reported advanced catalysts. When 2D Cu₂Zn₁Al_0.5Ce₅Zr_0.5O_x are applied to the photothermal CO₂ hydrogenation, it exhibits a record photochemical energy conversion efficiency of 36.2%, with a CO generation rate of 248.5 mmol g⁻¹ h⁻¹ and 571 L of CO yield under ambient sunlight irradiation. The high-entropy 2D materials provide a new route to simultaneously achieve catalytic stability and activity, greatly expanding the application boundaries of photothermal catalysis.

铜基纳米催化剂是各种工业催化过程的基石。协同增强铜基纳米催化剂的催化稳定性和活性是一项持续的挑战。在此，应用高熵原理修饰铜基纳米催化剂的结构，发明了一种 PVP 模板化方法，用于普遍合成 6-11 异种元素作为高熵二维 (2D) 材料。以2D Cu ₂ Zn ₁ Al _0.5 Ce ₅ Zr _0.5 O _x为例，其高熵结构不仅增强了400 ℃至800 ℃的耐烧结性，还提高了其CO ₂500 °C 下纯 CO 产率为 417.2 mmol g ^-1 h ^-1的氢化活性，比报道的先进催化剂高 4 倍。当二维Cu ₂ Zn ₁ Al _0.5 Ce ₅ Zr _0.5 O _x应用于CO ₂光热加氢时，其光化学能量转化效率达到创纪录的36.2%，CO生成率为248.5 mmol g ⁻¹ h ⁻¹在环境阳光照射下产生 571 L CO。高熵二维材料为同时实现催化稳定性和活性提供了一条新途径，极大地扩展了光热催化的应用边界。