Supported High‐Entropy Alloys for Electrooxidation of Benzyl Alcohol Assisted Water Electrolysis

Abstract Electrocatalytic hydrogen production technology is essentially vital for future green and sustainable energy revolution while its large‐scale industrial application is still unsatisfactory due to the low efficiency of electrocatalysts and kinetically sluggish oxygen evolution reaction (OER). Developing novel electrocatalysts and coupling them with upgrading organic molecules are considered effective solutions. Herein, it reports a high‐entropy composite electrocatalyst consisting of FeCoNiAlMo alloy and carbon nanotube (CNT) for anodic benzyl alcohol (BA) electrooxidation coupled with cathodic hydrogen production. Because of the lower charge transfer resistance and faster reaction kinetics, the quinary FeCoNiAlMo/CNT is highly active to OER, remarkably outperforming the ternary FeCoNi/CNT counterpart. Then, the FeCoNiAlMo/CNT composite electrocatalyst is further utilized for BA oxidation reaction‐assisted hydrogen evolution. Combining the experimental and calculation results, the different activities when tested in BA‐containing or BA‐free electrolytes can be attributed to the different metal active sites with specific surface adsorption effects to water and BA molecules, respectively. This work develops a novel electrocatalyst for high‐efficient alcohol oxidation‐assisted electrolysis.