Catalytically Active Au Layers Grown on Pd Nanoparticles for Direct Synthesis of H₂O₂: Lattice Strain and Charge-Transfer Perspective Analyses

Abstract

Despite its effectiveness in improving the properties of materials, strain engineering has not yet been employed to endow catalytic characteristics to apparently nonactive metals. This limitation can be overcome by controlling simultaneously lattice strains and charge transfer originated from the epitaxially prepared bimetallic core−shell structure. Here, we report the experimental results of the direct H 2 O 2 synthesis enabled by a strained Au layer grown on Pd nanoparticles. This system can benefit the individual catalytic properties of each involved material, and the heterostructured catalyst displays an improved productivity for the direct synthesis of H 2 O 2 by ∼100% relative to existing Pd catalysts. This is explained here by exploring the individual effects of lattice strain and charge transfer on the alteration of the electronic structure of ultrathin Au layers grown on Pd nanoparticles. The approach used in this study can be viewed as a means of designing catalysts with multiple catalytic functions.

Mechanical Reshaping of Inorganic Nanostructures with Weak Nanoscale Forces

“…37,38 Furthermore, the gradient of strained bonds in these materials has implications for their performance or study in catalytic systems. [33][34][35]39 Overall, this work demonstrates that inorganic nanoparticles may be thought of as being capable of dynamic structural changes, actuated by simple and ubiquitous nanoscale forces.…”

“…[30][31][32] It is worth noting that there still exist regions of elastically-strained bonds throughout the structure that are consistent with what has been observed to transform a normally inactive noble metal surface to one that can catalyze chemical reactions. [33][34][35] This suggests that such curvilinear nanostructures might have a high density of active sites for catalysis. In traditional nanoscale systems, there are canonical structures from which more complex architectures can be built (e.g., spheres assembled into a superlattice or rods lithographically fabricated into metamaterial arrays).…”

Mechanical Reshaping of Inorganic Nanostructures with Weak Nanoscale Forces

“…31,32 Furthermore, the gradient of strained bonds in these materials has implications for their performance or study in catalytic systems. 28,33 Overall, this work demonstrates that inorganic nanoparticles may be thought of as being capable of dynamic structural changes, actuated by simple and ubiquitous nanoscale forces.…”

“…[25][26][27] It is worth noting that there still exist regions of elastically-strained bonds throughout the structure that are consistent with what has been observed to transform a normally inactive noble metal surface to one that can catalyze chemical reactions. 28 This suggests that such curvilinear nanostructures might have a high density of active sites for catalysis. In traditional nanoscale systems, there are canonical structures from which more complex architectures can be built (e.g., spheres assembled into a superlattice, rods lithographically fabricated into metamaterial arrays, curved arms lithographically fabricated into a pinwheel).…”

Advanced Development Strategy of Nano Catalyst and DFT Calculations for Direct Synthesis of Hydrogen Peroxide

“…Palladium‐based bimetallic catalysts were investigated for the development of next‐generation catalysts. The literatures report the following categories of catalyst: noble‐metal‐containing bimetallic systems, such as PdPt, PdAu, and PdAg; [ 35–38 ] those with uncommon metal components, such as PdTe, PdSn, PdIn, and PdGa; [ 12,39–44 ] and transition‐metal‐based systems, such as PdCo, PdNi, and PdNiO. [ 45–47 ] Among them, there is no doubt that the PdAu bimetallic system is the most well‐known and prominent composition.…”