Although the unique properties of nanomaterials have endowed enzyme-mimic catalysts with broad applications, the development of catalysts still relies on trial-and-error strategies without predictive indicators. Surface electronic structures have rarely… Click to show full abstract
Although the unique properties of nanomaterials have endowed enzyme-mimic catalysts with broad applications, the development of catalysts still relies on trial-and-error strategies without predictive indicators. Surface electronic structures have rarely been studied in enzyme-mimic catalysts. Herein, we present a platform for understanding the impact of surface electronic structures on electrocatalysis toward H2O2 decomposition, using the Pd icosahedra (Pd ico), Pd octahedra (Pd oct) and Pd cubic nanocrystals as electrocatalysts. The electronic properties on Pd were modulated with a correlation of surface orientation. We revealed the relationship between the electronic properties and electrocatalytic performance, in which the surface electron accumulation can boost the electrocatalytic activity of the enzyme-mimic catalysts. As a result, the Pd icodimer exhibits the highest electrocatalytic and sensing efficiency. This work offers new perspectives for the investigation of structure-activity relationships and provides an effective knob for utilizing the surface electronic structures to boost the catalytic performance for enzyme-mimics.
               
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