Simultaneous Oxidative Cleavage of Lignin and Reduction of Furfural via Efficient Electrocatalysis by P‐Doped CoMoO ₄

Abstract Electrochemical oxidative lignin cleavage and coupled 2‐furaldehyde reduction provide a promising approach for producing high‐value added products. However, developing efficient bifunctional electrocatalysts with noble‐metal‐like activity still remains a challenge. Here, an efficient electrochemical strategy is reported for the selective oxidative cleavage of C _α –C _β bonds in lignin into aromatic monomers by tailoring the electronic structure through P‐doped CoMoO ₄ spinels (99% conversion, highest monomer selectivity of 56%). Additionally, the conversion and selectivity of 2‐furaldehyde reduction to 2‐methyl furan reach 87% and 73%, respectively. In situ Fourier transform infrared and density functional theory analysis reveal that an upward shift of the E _d upon P‐doping leads to an increase in the antibonding level, which facilitates the C _α –C _β adsorption of the lignin model compounds, thereby enhancing the bifunctional electrocatalytic activity of the active site. This work explores the potential of a spinel as a bifunctional electrocatalyst for the oxidative cracking of lignin and the reductive conversion of small organic molecules to high‐value added chemicals via P‐anion modulation.