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Engineering surface structure of Pt nanoshells on Pd nanocubes to preferentially expose active surfaces for ORR by manipulating the growth kinetics.

Nano Letters 2019 Februrary 6
Synthesis of Pt nanoshells on substrates can increase the utilization efficiency of Pt atoms and reduce the amount of Pt required in a process where it is essential. However, the growth of Pt nanoshells still faces challenges in tailoring the exposed crystal facets with which to control their catalytic activity and selectivity on a given substrate. In this work, we demonstrate a simple and convenient method capable for generating Pt octahedral islands with tunable sizes and densities on Pd cubic seeds by manipulating the deposition rate, which could be easily implemented and potentially applied to other noble metals. The success of this synthesis mainly relies on the fine control over the deposition rate. Due to the different reactivities at the surface sites, the deposition of Pt atoms can be controlled at a certain site by carefully tune the deposition rate. With a low concentration of reductant (8.33 mg/mL of glucose), surface diffusion dominates the process, resulting in the formation of Pt cubic shells on Pd cubic seeds. In contrast, when a higher amount of the reductant (16.67 mg/mL of glucose) is added, the deposition starts to dominate the overgrowth of Pt shells. In this case, the deposition of Pt would mainly occur at the corners of a cubic seed, resulting in the formation of eight large Pt octahedra on the surface of a Pd nanocube. Further increasing the deposition rate can result in much higher deposition rates, in which case, the deposition of Pt would likely to take place not only at the corners of a cubic seed, but also the edge and surface sites of the seeds. Not surprisingly, this growth habit can directly induce the formation of high-density octahedral islands on the surfaces of Pd cubic seeds. With the same amount of precursor supply, the higher densities of Pt islands, the smaller the size of the octahedral islands on Pd nanocubes. Unlike other synthetic methods, the size of the octahedral islands on Pd seeds can be even controlled to be smaller than 3 nm by simply controlling the amount of the Pt precursor. Considering the excellent performance of {111} facets of Pt catalysts toward ORR, the Pt nanocages with small octahedral islands on the surfaces can exhibit a high activity, with a mass activity 0.68 A/mg, as high as 5.2 times of that of commercial Pt/C.

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