Three-in-One Strategy to Improve Both Catalytic Activity and Selectivity: Nonconcentric Pd–Au Nanoparticles

Abstract

In direct H 2 O 2 synthesis, the Pd−Au alloy was considered as a potential catalyst because of its much better performance compared to the prototype Pd; unfortunately, achieving both high activity and selectivity remains a challenge. Here, we synthesized nonconcentric Pd−Au NPs in which Au domain shells are formed only partially on Pd domain cores and tested them for direct H 2 O 2 synthesis. It has three exposed regions of Pd, Au domains, and Pd−Au interfaces in a single NP (hence, a 3-in-1 strategy). Creating nonconcentric forms was demonstrated convincingly by density functional theory calculations. The nonconcentric Pd−Au particles exhibit high and well-balanced performances that are hard to achieve with traditional alloyed Pd−Au. The number of Pd/Au interfaces was found to be the key factor and thus was optimized by controlling the Au precursor concentrations. The hitherto underutilized structure of nonconcentric bimetallic alloys can be useful and thus should be more actively investigated for catalyst development.

Colloidal Synthesis of Metal Nanocrystals: From Asymmetrical Growth to Symmetry Breaking

“…Copyright 2012 American Chemical Society. (B) Adapted with permission from ref . Copyright 2021 American Association for the Advancement of Science.…”

“…With knowledge of each parameter’s role in kinetic control, a recent study further simplified the protocol for the synthesis of nonconcentric nanocubes (Figure B) . Instead of adding the solution dropwise with the assistance of a syringe pump, the V dep of Au atoms on cubic Pd seeds was controlled by simply varying the amount of Au precursor in the reaction mixture.…”

“…With knowledge of each parameter's role in kinetic control, a recent study further simplified the protocol for the synthesis of nonconcentric nanocubes (Figure 24B). 297 Instead of adding Beyond the limited supply of precursor, oxidative etching is another effective strategy for breaking the symmetry of cubic nanocrystals. Similar to the case of Pd truncated octahedral seeds, the asymmetrical growth of Br − -capped Pd cubes could be triggered on one of the six side faces due to localized surface activation through oxidative etching.…”

Plating of Ion‐Exchange Membranes: A Molecular Dynamics Study

“…Ionic conductivity, σ c , was calculated following ref. [74] and using the Nernst–Einstein relation, $$$$\begin{equation} \sigma _{\mathrm{c}} = \frac{Ne^2}{VTk_{\mathrm{B}}}D_{\mathrm{tot}} \end{equation}$$$$where N is the number of counterions, $$e=1.602 \times {10}^{-19}\hspace*{0.16666666666666666em}\mathrm{C}$$ is the universal charge, V is the average system volume, $$T=303.15\hspace*{0.16666666666666666em}\mathrm{K}$$ is the temperature, $${k}_{\mathrm{B}}=1.381 \times {10}^{-23}\hspace*{0.16666666666666666em}{\mathrm{m}}^{2}\hspace*{0.16666666666666666em}\mathrm{kg}\hspace*{0.16666666666666666em}{\mathrm{s}}^{-2}\hspace*{0.16666666666666666em}{\mathrm{K}}^{-1}$$ is the Boltzmann constant, and D tot is the self‐diffusion coefficient.…”

S-Scheme Heterojunction Photocatalysts for H2O2 Production

“…Another popular method is the direct synthesis from H 2 and O 2 using Pd-and Au-based catalysts. 6 However, the O 2 and H 2 feed gases must be thoroughly diluted with inert gases to avoid explosion, resulting in low H 2 O 2 productivity. Also, this route suffers from low H 2 O 2 selectivity and fast H 2 O 2 decomposition.…”