LAUSR

Medium‐entropy alloy aerogels (MEAAs) with the advantages of both multimetallic alloys and aerogels are promising new materials in catalytic applications. However, limited by the immiscible behavior of different metals, achieving single‐phase MEAAs is still a grand challenge. Herein, a general strategy for preparing ultralight 3D porous MEAAs with the lowest density of 39.3 mg cm−3 among the metal materials is reported, through combining auto‐combustion and subsequent low‐temperature reduction procedures. The homogenous mixing of precursors at the ionic level makes the short‐range diffusion of metal atoms possible to drive the formation of single‐phase MEAAs. As a proof of concept in catalysis, as‐synthesized Ni50Co15Fe30Cu5 MEAAs exhibit a high mass activity of 1.62 A mg−1 and specific activity of 132.24 mA cm−2 toward methanol oxidation reactions, much higher than those of the low‐entropy counterparts. In situ Fourier transform infrared and NMR spectroscopies reveal that MEAAs can enable highly selective conversion of methanol to formate. Most importantly, a methanol‐oxidation‐assisted MEAAs‐based water electrolyzer can achieve a low cell voltage of 1.476 V at 10 mA cm−2 for making value‐added formate at the anode and H2 at the cathode, 173 mV lower than that of traditional alkaline water electrolyzers.