Effective immobilization of nanoscale Pd on a carbon hybrid for enhanced electrocatalytic performances: stabilization mechanism investigations

摘要

The grand challenge inhibiting the use of electrocatalysts is the degradation of active species which results in poor durability and long-term performances. Studying the origin of active metal particle stabilization mechanisms by using supports and the immobilization-induced changes of active particles is of significant importance. This study describes the preparation of Pd nanoparticles supported by carbon hybrid NPG-CN, revealing that the mass and specific activities (1987 A g(-1) Pd and 28.7 A m(-2)) of this catalyst for formic acid oxidation significantly exceed those of commercial Pd/C, and excellent stability and enhanced CO-poisoning tolerance properties are obtained. The origin of this behavior is probed by surface analytical techniques and identical-location transmission electron microscopy (IL-TEM), and the enhanced activity of Pd/NPG-CN is ascribed to the electronic effect of the substrate, the high content of surface metallic Pd-0, and the reduced extent of active Pd leaching and physical ripening during the FOA process compared with commercial Pd/C. In addition, theoretical calculations demonstrate that NPG-CN can efficiently trap Pd atoms, which accumulate and form Pd clusters at trapping (nucleation) sites.