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Effect of size and oxidation state of platinum nanoparticles on the electrocatalytic performance of graphene-nanoparticle composites

机译:铂纳米粒子的尺寸和氧化态对石墨烯-纳米粒子复合材料电催化性能的影响

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摘要

A surfactant and stabilizer free graphene-based composite with Pt nanoparticles is considered to be a promising electrocatalyst with greatly improved performance. Here we show that both the size and oxidation state of Pt nanoparticles can significantly influence the electrocatalytic performance of the nanocomposite. We have synthesized Pt-graphene nanocomposites with varied sizes and oxidation states of Pt nanoparticles and test their catalytic activity towards methanol electro-oxidation. We found that the size <1.5 nm with mixed oxidation offers methanol oxidation at lower onset potential and with better tolerance to CO poisoning. However, these benefits are lost due to catalyst durability and thus catalytic current decays rapidly with time. As the nanoparticle size increases in the range of 2-5 nm this onset potential increases, CO tolerance decreases but the catalytic current becomes more stable with time. Thus an optimum nanoparticle size of 2.2 nm shows the best catalytic activity and durability. The oxygenic platinum with variable oxidation states offers stable grafting with the graphene surface, prevents active Pt (0) sites and assists for better CO tolerance. This result would be useful in the design and development of electrocatalysts with better performances.
机译:具有Pt纳米粒子的无表面活性剂和无稳定剂的石墨烯基复合材料被认为是一种有望大大改善其性能的电催化剂。在这里我们表明,Pt纳米颗粒的大小和氧化态都可以显着影响纳米复合材料的电催化性能。我们已经合成了具有不同大小和Pt纳米粒子氧化态的Pt-石墨烯纳米复合材料,并测试了它们对甲醇电氧化的催化活性。我们发现,混合氧化<1.5 nm时,甲醇的氧化起始电位较低,对CO中毒的耐受性更好。但是,由于催化剂的耐用性,这些益处丧失了,因此催化电流随时间迅速衰减。随着纳米颗粒尺寸在2-5 nm范围内增加,此起始电位增加,CO耐受性降低,但催化电流随时间变得更稳定。因此,2.2nm的最佳纳米颗粒尺寸显示出最佳的催化活性和耐久性。具有可变氧化态的含氧铂提供了与石墨烯表面的稳定接枝,防止了活性Pt(0)的位点并有助于获得更好的CO耐受性。该结果将对具有更好性能的电催化剂的设计和开发有用。

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