In Situ Patterning of Nickel/Sulfur-codoped Laser-induced Graphene Electrode for Selective Electrocatalytic Valorization of Glycerol

The electrocatalytic valorization of glycerol is an emerging upcycling process for the biomass utilization. In this work, nickel/sulfur-codoped laser-induced graphene (LINiSG) on flexible polyimide film was fabricated and demonstrated as a self-supported and binder-free monolithic electrode for electrocatalytic glycerol oxidation reaction (EGOR) towards the selective generation of value-added three-carbon (C3) chemicals. The laser-induced in-situ and synchronous carbonization of polysulfone and Ni precursor was demonstrated to remarkably promote both the electrochemical surface area and Ni loading of LINiSG electrode. These synergistic merits are considered as the main origin for its enhanced EGOR activity and stability, showing much smaller Tafel slope and 2-fold enhanced current density, as compared to LINiG electrode without the co-carbonization of polysulfone. The influence of experimental parameters has been systematically investigated by the product analysis, achieving an average 94.7% C3 selectivity and 76.1% C3 Faradaic efficiency with a high selectivity of dihydroxyacetone (ca. 67.7%) in near-neutral conditions, which is better than most of the reported EGOR electrodes operated in near-neutral conditions. This work demonstrated the viability of using flexible self-supported and binder-free LIG electrode with rational design and preparation approach for electrocatalytic valorization of biomass.