Nitrogen-doped graphene stabilized gold nanoparticles for aerobic selective oxidation of benzylic alcohols

Nitrogen-doped graphene stabilized gold nanoparticles for aerobic selective oxidation of benzylic alcohols
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氮掺杂石墨烯稳定金纳米粒子用于苯甲醇的有氧选择性氧化

DOI:
10.1039/c2ra21291a
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发表时间:
2012-11
期刊:
影响因子:
3.9
通讯作者:
Wang Xuxu
Wang Xuxu
中科院分区:
化学3区
文献类型:
--
作者:
Zhang Zizhong;Zhang Zizhong;Wang Xuxu;Wang Xuxu

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由于石墨烯和金的独特性质,人们越来越多地致力于制备Au/石墨烯复合材料。利用还原氧化石墨烯(RGO)上的含氧官能团作为纳米颗粒的“拴系柱”,将平均粒径为几十纳米的Au纳米颗粒直接沉积在RGO上。一些官能团,如氨基和硫醇,连接到石墨烯的表面,以稳定具有较小粒径(一般<5 nm)的金纳米粒子。不幸的是,这些策略中的大多数导致Au颗粒具有有限的暴露原子,这对于它们的应用(例如催化)肯定是不利的。氮杂原子的引入不仅可以调节石墨烯的电子结构,而且可以改变石墨烯的表面性质。采用直接简单还原法在氮掺杂石墨烯纳米片(NG)上制备了平均粒径为2-4 nm的裸Au纳米粒子。采用XRD、XPS、TEM、AFM和拉曼光谱对Au/NG纳米复合材料进行了表征。结果表明,掺杂在NG中的氮原子,而不是缺陷或氧部分,在稳定Au NPs中起着至关重要的作用。研究还发现,在Au/NG催化剂上苯甲醇氧化的初始反应速率比在Au/石墨烯催化剂上高约10倍。我们的研究结果可能提供一个线索,氮掺入稳定未封顶的贵金属纳米粒子的石墨烯或其他无机氧化物载体,如二氧化钛。
Increasing efforts have been made to fabricate Au/graphene composites due to the fascinating properties of both graphene and gold. Some Au nanoparticles with an average size of tens of nanometers were directly deposited on reduced graphene oxide (RGO), utilizing the residual oxy-functional groups as the “hitching post” of the nanoparticles. Some functional groups, such as amino and thiol, were attached to the surface of the graphene in order to stabilize gold nanoparticles with a smaller particle size (<5 nm in general). Unfortunately, most of these strategies result in Au particles with limited exposed atoms, which is certainly a disadvantage for their application, such as catalysis. Introduction of nitrogen heteroatoms into the framework of graphene can not only modulate the electronic structure, but also change the surface properties of the graphene. In this work, naked Au nanoparticles with an average size of about 2–4 nm were fabricated on nitrogen-doped graphene nanosheets (NG) via the direct simple reduction method. The Au/NG nanocomposites were characterized by XRD, XPS, TEM, AFM and Raman. It was revealed that the nitrogen atoms doped in NG, rather than defects or oxygen moieties, play an essential role in stabilizing Au NPs. It was also found that the initial reaction rate of benzyl alcohol oxidation over the Au/NG catalyst is about ten fold higher than that over Au/graphene catalysts. Our findings may provide a clue of nitrogen incorporation to stabilize uncapped noble metal nanoparticles on graphene or other inorganic oxide supports, such as TiO2.
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