One-pot synthesis of core-shell Cu@SiO2 nanospheres and their catalysis for hydrolytic dehydrogenation of ammonia borane and hydrazine borane.

One-pot synthesis of core-shell Cu@SiO2 nanospheres and their catalysis for hydrolytic dehydrogenation of ammonia borane and hydrazine borane.
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一锅法合成核壳Cu@SiO2纳米球及其催化氨硼烷和肼硼烷水解脱氢

DOI:
10.1038/srep07597
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发表时间:
2014-12-23
期刊:
影响因子:
4.6
通讯作者:
Lan Y
Lan Y
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Yao Q;Lu ZH;Zhang Z;Chen X;Lan Y

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采用反胶束体系一锅法制备了多孔SiO2纳米球(Cu@SiO2)包裹的超细铜纳米粒子(Cu NPs),并用SEM、TEM、EDX、XRD、N2吸附-脱附、CO-TPD、XPS和ICP等方法对其进行了表征。表征结果表明,直径约为2 nm的超细Cu NPs有效地嵌入直径约为25 nm的均匀球形SiO2 NPs的中心。  与商业化的SiO2负载Cu纳米颗粒、SiO2纳米球负载Cu纳米颗粒和游离Cu纳米颗粒相比,所合成的核-壳纳米球Cu@SiO2在室温下对氨硼烷(AB,NH3 BH 3)和肼硼烷(HB,N2 H4 BH 3)的水解脱氢反应表现出上级催化活性。在Cu@SiO2纳米球的存在下,AB和HB水解的转换频率(TOF)分别为3.24和7.58 mol H2(mol Cu min)-1,在相同的反应中,Cu纳米催化剂的转换频率相对较高。 此外,循环测试表明,Cu@SiO2纳米球在AB和HB的水解中仍然具有高活性,即使在十次循环后,仍分别保持其初始催化活性的90%和85%。
Ultrafine copper nanoparticles (Cu NPs) within porous silica nanospheres (Cu@SiO2) were prepared via a simple one-pot synthetic route in a reverse micelle system and characterized by SEM, TEM, EDX, XRD, N2 adsorption-desorption, CO-TPD, XPS and ICP methods. The characterized results show that ultrafine Cu NPs with diameter of around 2 nm are effectively embedded in the center of well-proportioned spherical SiO2 NPs of about 25 nm in diameter. Compared to commercial SiO2 supported Cu NPs, SiO2 nanospheres supported Cu NPs and free Cu NPs, the synthesized core-shell nanospheres Cu@SiO2 exhibit a superior catalytic activity for the hydrolytic dehydrogenation of ammonia borane (AB, NH3BH3) and hydrazine borane (HB, N2H4BH3) under ambient atmosphere at room temperature. The turnover frequencies (TOF) for the hydrolysis of AB and HB in the presence of Cu@SiO2 nanospheres were measured to be 3.24 and 7.58 mol H2 (mol Cu min)−1, respectively, relatively high values for Cu nanocatalysts in the same reaction. In addition, the recycle tests show that the Cu@SiO2 nanospheres are still highly active in the hydrolysis of AB and HB, preserving 90 and 85% of their initial catalytic activity even after ten recycles, respectively.
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