碱基调控Pt纳米晶的构型及其催化加氢性能研究
首发时间:2016-06-27
摘要:催化加氢反应具有原子经济性、产品质量好、后处理容易以及反应选择性可控制的优点,使其成为处理石油化工产品的重要手段。Pt纳米晶对加氢反应具有良好的催化性能,其催化活性和选择性与纳米晶的形貌和尺寸密切相关。由Gibbs-Wulff晶体生长定律可知,通过加入特定结构封端剂可以有效控制纳米晶的尺寸和形貌。本文采用NaBH4在溶液中还原Pt的前驱体H2PtCl6的方法制备Pt纳米晶,并将其用于对硝基苯酚(p-NIP)的还原反应。实验系统研究了碱基分子(如腺嘌呤A、鸟嘌呤G、胸腺嘧啶T、胞嘧啶C及对应的核苷)对Pt纳米晶构型和催化加氢活性的调控规律。研究发现,碱基生物分子对于Pt纳米晶的形貌以及尺寸具有明显的调控作用,通过不同结构碱基分子的精密调控,实验制备得到了形貌和尺寸各异的Pt纳米晶。同时,所得Pt纳米晶在p-NIP的加氢反应评价中表现出了精密可调的催化性能。调控剂分子的结构对于纳米晶的加氢性能有着直接的影响,核苷分子相比对应的碱基分子多了一分子核糖,其制备得到的纳米晶的加氢效果要优于碱基调控得到的纳米晶。
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DNA-base regulation of Pt nanocrystals: morphology and catalytic activity for hydrogenation
Abstract:Catalytic hydrogenation is one of the important means for processing petroleum chemical products because of its atomic economy, good product quality, easy post-processing, and controllable selectivity. Pt nanoparticles (NPs) have been used as the catalyst for many hydrogenation reactions due to their good catalytic performance. Their catalytic activity and selectivity are strongly depended on their size and morphology. According to Gibbs-Wulff theory, the morphology and size of NPs can be effectively controlled by certain capping agent. In this paper, NaBH4 has been used to reduce platinum precursor (H2PtCl6) to prepare Pt NPs in water solution. The reduction of p-nitrophenol (p-NIP) by H2 was employed as model reaction to evaluate catalytic performance of as-prepared Pt NPs. Various biomolecules, including DNA basic groups (adenine, guanine, thymine, cytosine) and corresponding nucleosides, were chosen as capping agent to control the size and shape of Pt NPs. Experimental results show that capping agents of biological molecules have apparent effect on the regulation of Pt NPs. Pt NPs with multiple morphologies and sizes have been successfully prepared. Simultaneously, the as-prepared catalysts showed precisely controllable activity for the hydrogenation of p-NIP. The structure of biomolecule has a direct impact on the catalytic performance of the catalyst. The Pt NPs regulated by nucleoside exhibit much higher activity than that of corresponding DNA-base, which could be ascribed to the presence of extra ribose molecule in nucleosides.
Keywords: Chemical technology Pt nanoparticles catalytic hydrogenation DNA base
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