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Hydrogen Evolution Linked to Selective Oxidation of Glycerol over CoMoO4—A Theoretically Predicted Catalyst

Electrochemical valorization of biomass waste (e.g., glycerol) for production of value‐added products (such as formic acid) in parallel with hydrogen production holds great potential for developing renewable and clean energy sources. Here, a synergistic effort between theoretical calculations at the atomic level and experiments to predict and validate a promising oxide catalyst for the glycerol oxidation reaction (GOR) are reported, providing a good example of designing novel, cost‐effective, and highly efficient electrocatalysts for producing value‐added products at the anode and high‐purity hydrogen at the cathode. The predicted CoMoO4 catalyst is experimentally validated as a suitable catalyst for GOR and found to perform best among the investigated metal (Mn, Co, Ni) molybdate counterparts. The potential required to reach 10 mA cm−2 is 1.105 V at 60 °C in an electrolyte of 1.0 m KOH with 0.1 m glycerol, which is 314 mV lower than for oxygen evolution. The GOR reaction pathway and mechanism based on this CoMoO4 catalyst are revealed by high‐performance liquid chromatography and in situ Raman analysis. The coupled quantitative analysis indicates that the CoMoO4 catalyst is highly active toward CC cleavage, thus presenting a high selectivity (92%) and Faradaic efficiency (90%) for formate production.