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Modulation of bimetallic nanocatalysts with atomic precision would allow for significant increases in catalyst activity through the optimization of heteroatomic interplay. In practice, this level o...

Advances in new systems of organic–inorganic hybrid nanocomposites are less prevalent, owing to a lack of facile strategies for precise control of their structures, compositions, and, hence, their properties. In this work, Au-BINOL hybrid nanocomposites with eccentric and concentric nanostructures were produced. The hybrid nanocomposites containing two distinct moieties of inorganic Au nanocrystals and organic BINOL nanospheres were applied to the catalytic hydrogenation of 4-nitrophenol with NaBH4 in the aqueous phase with and without the illumination of visible light. Here, we demonstrate that the existence of Au–BINOL interfaces offers benefits to their performance. The eccentric nanostructures made with CTAC show the superior activity from large Au–BINOL interfaces formed between the BINOL nanospheres and the faces of Au nanoplates. They further exhibit a high Au localized surface plasmon resonance (LSPR)-enhancement effect on the photoreduction of 4-nitrophenol, which is attributed to the strong LSPR...

We investigated lattice strain on alloyed surfaces using ∼10 nm core–shell nanoparticles with controlled size, shape, and composition. We developed a wet-chemistry method for synthesizing small octahedral PdPt alloy nanoparticles and Au@PdPt core–shell nanoparticles with Pd–Pt alloy shells and Au cores. Upon introduction of the Au core, the size and shape of the overall nanostructure and the composition of the alloyed PdPt were maintained, enabling the use of the electrooxidation of formic acid as a probe to compare the surface structures with different lattice strain. We have found that the structure of the alloyed surface is indeed impacted by the lattice strain generated by the Au core. To further reveal the impact of lattice strain, we fine-tuned the shell thickness. Then, we used synchrotron-based X-ray diffraction to investigate the degree of lattice strain and compared the observations with the results of the formic acid electrooxidation, suggesting that there is an optimal intermediate shell thickness for high catalytic activity.

The combined functionality of components in organic–inorganic hybrid nanomaterials render them efficient nanoreactors. However, the development in this field is limited due to a lack of synthetic avenues and systematic control of the growth kinetics of hybrid structures. In this work, we take advantage of an ionic switch for regio-control of Au-BINOL(1,1′-Bi-2-naphthol) hybrid nanostructures. Aromatic BINOL molecules assemble into nanospheres, concomitant with the growth of the Au nanocrystals. The morphological evolution of Au nanocrystals is solely controlled by the presence of halides in the synthetic system. Here we show that quaternary ammonium surfactants (CTAB or CTAC), not only bridging Au and BINOL, but also contributing to the formation of concentric or eccentric structures when their concentrations are tuned to the range of 10–5 to 10–3 M. This facile strategy offers the potential advantage of scalable production, with diverse functional organic–inorganic hybrid nanocomposites being produced ba...

Control of morphology in the synthesis of Rh nanocrystals can be used to precisely tailor the electronic surface structure; this in turn directly influences their performance in catalysis applications. Many works bring attention to the development of Rh nanostructures with low-index surfaces, but limited effort has been placed on the study of high-index and surface-defect-enriched nanocrystals as they are not favored by thermodynamics due to the involvement of high-energy surfaces and increased surface-to-volume ratios. In this work, we demonstrate an aqueous synthesis of concave Rh nanotetrahedra (CTDs) serving as efficient catalysts for energy conversion reactions. CTDs are surface-defect-rich structures that form through a slow growth rate and follow the four-step model of metallic nanoparticle growth. By tuning the surfactant concentration, the morphology of Rh CTDs evolved into highly excavated nanotetrahedra (HETDs) and twinned nanoparticles (TWs). Unlike the CTD surfaces with abundant adatoms and v...

Conventional gas sensors work upon changes in mechanical or conductive properties of sensing materials during a chemical process, which may limit availabilities of size miniaturization and design simplification. However, fabrication of miniaturized sensors with superior sensitivities in real-time and label-free probing of chemical reactions or catalytic processes remains highly challenging, in particular with regard to integration of materials into a desired smaller volume without losing the recyclability of sensing properties. Here, we demonstrate a unique bimetallic nanostructure, the Au–Pd–Au core–shell–frame nanobrick, as a promising archetype for fabrication of miniaturized sensors at nanoscale. Upon analysis of the aqueous synthesis, both ex situ and in situ, the formation of Au frames is consistent with selective deposition and aggregation of NaBH4-reduced Au nanoparticles at the corners and edges of cubic Pd shells, where the {100} surfaces, capped by iodide ions, are growth-limited. By virtue of ...