RESUMO
Improving the electrocatalytic properties by regulating the surface electronic structure of supported metals has always been a hot issue in electrocatalysis. Herein, two novel catalysts Pd/B-N-Ti3C2 and Pd/N-B-Ti3C2 are used as the models to explore the effect of the B and N co-doping sequence on the surface electronic structure of metals, together with the electrocatalytic properties of ethanol oxidation reaction. The two catalysts exhibit obviously stratified morphology, and the Pd nanoparticles having the same amount are both uniformly distributed on the surface. However, the electron binding energy of Ti and Pd elements of Pd/B-N-Ti3C2 is smaller than that of Pd/N-B-Ti3C2. By exploring the electrocatalytic properties for EOR, it can be seen that all the electrochemical surface area, maximum peak current density, and antitoxicity of the Pd/B-N-Ti3C2 catalyst are much better than its counterpart. Such different properties of the catalysts can be attributed to the various doping species of B and N introduced by the doping sequence, which significantly affect the surface electronic structure and size distribution of supported metal Pd. Density functional theory calculations demonstrate that different B-doped species can offer sites for the H atom from CH3CH2OH of dehydrogenation in Pd/B-N-Ti3C2, thereby facilitating the progress of the EOR to a favorable pathway. This work provides a new insight into synthesizing the high-performance anode materials for ethanol fuel cells by regulating the supported metal catalyst with multielement doping.
