Overlayer Pt on Ni (Ni@Pt) or Co (Co@Pt) were synthesized and tested for H<
sub>
2<
/sub>
generation from APR of lactose. H<
sub>
2<
/sub>
chemisorption descriptor showed that Ni@Pt and Co@Pt overlayer catalysts had reduced H<
sub>
2<
/sub>
adsorption strength compared to a Pt only catalyst, which agree with computational predictions. The overlayer catalysts also demonstrated lower activity for ethylene hydrogenation than the Pt only catalyst, which likely resulted from decreased H<
sub>
2<
/sub>
binding strength decreasing the surface coverage of H<
sub>
2<
/sub>
. XAS results showed that overlayer catalysts exhibited higher white line intensity than the Pt catalyst, which indicates a negative d-band shift for the Pt overlayer, further providing evidence for overlayer formation. Lactose APR studies showed that lactose can be used as feedstock to produce H<
sub>
2<
/sub>
and CO under desirable reaction conditions. The Pt active sites of Ni@Pt and Co@Pt overlayer catalysts showed significantly enhanced H<
sub>
2<
/sub>
production selectivity and activity when compared with that of a Pt only catalyst. The single deposition overlayer with the largest d-band shift showed the highest H<
sub>
2<
/sub>
activity. Here, the results suggest that overlayer formation using directed deposition technique could modify the behavior of the surface metal and ultimately modify the APR activity.