Steering the activity and selectivity of liquid fuels electro-oxidation via molecule in-situ modification of Pt

The catalytic efficiency of the formic acid electro-oxidation reaction (FAOR) and glycerol electro-oxidation reaction (GOR) using a Pt catalyst was substantially enhanced by adding 7,7,8,8-tetracyanoquinodimethane (TCNQ) dissolved in acetonitrile solution (ACN) into the reaction solution. The dynamic structure of TCNQ(ACN) and blank ACN modified Pt catalysts, along with their impacts on the performances in FAOR and GOR were analyzed. A strong relationship was established between the performance of FAOR and GOR and the modifier concentration in the reaction solution. ACN exerted a geometric blocking effect on Pt, thereby considerably improving the direct dehydrogenation process of FAOR. Based on ACN, the performance of the dehydrogenation process of FAOR and GOR was further boosted for the surface electron-rich Pt catalyst due to modification with additional TCNQ modifier. Additionally, the resistance to CO poisoning of modified Pt catalyst was notably improved, and the onset potential decreased from 0.656 V of the unmodified Pt to 0.583 V for a specific amount of TCNQ(ACN) modified Pt catalyst. This study offers a novel perspective to optimize the catalytic performance of the catalyst.