To obtain high catalytic properties, finely modulating the electronic structure and active sites of catalysts is important. Herein, we report the design and economical synthesis of Pd@Pt core–shell nanoparticles for high productivity in the direct synthesis of hydrogen peroxide. Pd@Pt core–shell nanoparticles with a partially covered Pt shell on a Pd cube were synthesized using a simple direct seed-mediated growth method. The synthesized Pd@Pt core–shell nanoparticles were composed of high index faceted Pt on the corners and edges, while the Pd–Pt alloy was located on the terrace area of the Pd cubes. Because of the high-indexed Pt and Pd–Pt alloy sites, the synthesized concave Pd@Pt7 nanoparticles exhibited both high H2 conversion and H2O2 selectivity compared with Pd cubes.

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.

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Hydrogen peroxide is a simple oxidizing agent. Its environmental benignness and effectiveness have led to a continuous increase in its use and production. Anthraquinone autoxidation (the AO process) is generally used to manufacture hydrogen peroxide (H2O2); however, this complex multi‐stage process releases large amounts of organic solvent into the environment and requires significant energy to operate. As a green and energy‐efficient production method, the direct synthesis of hydrogen peroxide (DSHP) from molecular hydrogen and oxygen can overcome the disadvantages of the AO process. However, DSHP has remained challenging until recently as severe mass‐transfer limitations and unavoidable side reactions result in insufficient selectivity for H2O2. However, beyond the conventional development methods for catalysts, recent advances in chemical and engineering fields can appreciably assist in the discovery of a “dream catalyst” for DSHP; high‐end computational methods and the facile surface‐controllable syntheses of nanocatalysts. This review addresses how a combination of density functional theory (DFT) calculations and nanocatalyst synthesis technologies lead to the development of high‐performance catalysts for DSHP, and provides guidelines on efficient methodologies for the development of catalysts through the use of cutting edge technologies.

The catalytic properties of materials are determined by their electronic structures, which are based on the arrangement of atoms. Using precise calculations, synthesis, analysis, and catalytic activity studies, we demonstrate that changing the lattice constant of a material can modify its electronic structure and therefore its catalytic activity. Pd/Au core/shell nanocubes with a thin Au shell thickness of 1 nm exhibit high H2O2 production rates due to their improved oxygen binding energy (ΔE O) and hydrogen binding energy (ΔE H), as well as their reduced activation barriers for key reactions.

Addition of polyvinylpyrrolidone to Pd/SiO2 catalyst improved H2O2 selectivity by adjusting electronic state of palladium active species.

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