Regulating Surface Facets of Metallic Aerogel Electrocatalysts by Size-Dependent Localized Ostwald Ripening.

It is well known that the activity and stability of electrocatalysts are largely dependent on their surface facets. In this work, we have successfully regulated surface facets of three-dimensional (3D) metallic Au m- n aerogels by salt-induced assembly of citrate-stabilized gold nanoparticles (Au NPs) of two different sizes and further size-dependent localized Ostwald ripening at controlled particle number ratios, where m and n represent the size of Au NPs. In addition, 3D Au m- n-Pd aerogels were further synthesized on the basis of Au m- n aerogels and also bear controlled surface facets because of the formation of ultrathin Pd layers on Au m- n aerogels. Taking the electrooxidation of small organic molecules (such as methanol and ethanol) by the resulting Au m- n and Au m- n-Pd aerogels as examples, it is found that surface facets of metallic aerogels with excellent performance can be regulated to realize preferential surface facets for methanol oxidation and ethanol oxidation, respectively. Moreover, they also indeed simultaneously bear high activity and excellent stability. Furthermore, their activities and stability are also highly dependent on the area ratio of active facets and inactive facets on their surfaces, respectively, and these ratios are varied via the mismatch of sizes of adjacent NPs. Thus, this work not only demonstrates the realization of the regulation of the surface facets of metallic aerogels by size-dependent localized Ostwald ripening but also will open up a new way to improve electrocatalytic performance of 3D metallic aerogels by surface regulation.