Synergistic effect of PtNi alloy and N-doped carbon on selective electrocatalytic hydrogenation of phenol to cyclohexanone

Cyclohexanone is an essential intermediate in nylon production and serves as an effective solvent for resins. Electrocatalytic hydrogenation of phenol, a lignin derivative, provides a green and efficient route to cyclohexanone. However, developing catalysts that simultaneously achieve high selectivity, yield, and Faradaic efficiency for cyclohexanone remains a challenge. Here, we report an N-doped, hydrophilic carbon-supported PtNi alloy catalyst (PtNi/NC), which achieves 98% phenol conversion within 75 min, 93.8% cyclohexanone selectivity, and a Faradaic efficiency of 52.1% under mild conditions, and shows a low apparent activation energy of 31.6 kJ mol -1 . The superior catalytic activity and high selectivity are attributed to the synergistic effects of the PtNi alloy structure, N-doping carbon matrix, and improved hydrophilicity of the support. This work presents a rational design strategy for developing efficient electrocatalysts for the selective production of cyclohexanone and the valorization of lignin-derived phenolic compounds. Electrocatalytic hydrogenation of lignin-derived phenol to cyclohexanone proceeds efficiently over a PtNi/NC catalyst, where synergistic Pt–Ni sites promote surface-adsorbed hydrogen activation, enabling high conversion and selectivity under mild reaction conditions • Ni doping Pt tuned surface electronics to facilitate selective electrocatalytic hydrogenation of phenol to cyclohexanone • Nitrogen-doped carbon support improves catalyst dispersion and promotes cyclohexanone release • Interfacial synergy suppresses overhydrogenation and competing hydrogen evolution • Nearly complete phenol conversion is achieved under mild conditions with high cyclohexanone selectivity • The catalyst design offers an efficient route for upgrading lignin-derived phenolic compounds