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载于硅烷化钴铁氧体磁性颗粒上的铜(0)纳米粒子:在氨硼烷水解反应中具有成本效益的催化剂,具有优异的可重复使用性能。

Copper(0) nanoparticles supported on silica-coated cobalt ferrite magnetic particles: cost effective catalyst in the hydrolysis of ammonia-borane with an exceptional reusability performance.

机构信息

Department of Chemical Engineering and Applied Chemistry, Atilim University, 06836 Ankara, Turkey.

出版信息

ACS Appl Mater Interfaces. 2012 Aug;4(8):3866-73. doi: 10.1021/am3005994. Epub 2012 Aug 13.

DOI:10.1021/am3005994
PMID:22856878
Abstract

Herein we report the development of a new and cost-effective nanocomposite catalyst for the hydrolysis of ammonia-borane (NH(3)BH(3)), which is considered to be one of the most promising solid hydrogen carriers because of its high gravimetric hydrogen storage capacity (19.6% wt) and low molecular weight. The new catalyst system consisting of copper nanoparticles supported on magnetic SiO(2)/CoFe(2)O(4) particles was reproducibly prepared by wet-impregnation of Cu(II) ions on SiO(2)/CoFe(2)O(4) followed by in situ reduction of the Cu(II) ions on the surface of magnetic support during the hydrolysis of NH(3)BH(3) and characterized by ICP-MS, XRD, XPS, TEM, HR-TEM and N(2) adsorption-desorption technique. Copper nanoparticles supported on silica coated cobalt(II) ferrite SiO(2)/CoFe(2)O(4) (CuNPs@SCF) act as highly active catalyst in the hydrolysis of ammonia-borane, providing an initial turnover frequency of TOF = 2400 h(-1) at room temperature, which is not only higher than all the non-noble metal catalysts but also higher than the majority of the noble metal based homogeneous and heterogeneous catalysts employed in the same reaction. More importantly, they were easily recovered by using a permanent magnet in the reactor wall and reused for up to 10 recycles without losing their inherent catalytic activity significantly, which demonstrates the exceptional reusability of the CuNPs@SCF catalyst.

摘要

在这里,我们报告了一种新型且经济高效的纳米复合材料催化剂的开发,用于氨硼烷(NH(3)BH(3))的水解。由于其高重量比氢存储容量(19.6%wt)和低分子量,氨硼烷被认为是最有前途的固体储氢载体之一。由磁性 SiO(2)/CoFe(2)O(4)颗粒负载的铜纳米颗粒组成的新催化剂体系通过 Cu(II)离子在 SiO(2)/CoFe(2)O(4)上的湿浸渍以及在 NH(3)BH(3)水解过程中磁性载体表面上的 Cu(II)离子的原位还原来重复制备,并用 ICP-MS、XRD、XPS、TEM、HR-TEM 和 N(2)吸附-解吸技术进行了表征。负载在二氧化硅涂层的钴(II)铁(SiO(2)/CoFe(2)O(4)上的铜纳米颗粒(CuNPs@SCF)在氨硼烷的水解中作为高活性催化剂,在室温下提供初始周转率(TOF)= 2400 h(-1),不仅高于所有非贵金属催化剂,而且高于在相同反应中使用的大多数贵金属均相和多相催化剂。更重要的是,它们可以在反应器壁上使用永磁体轻松回收,并在不显着损失其固有催化活性的情况下重复使用多达 10 次循环,这证明了 CuNPs@SCF 催化剂的非凡可重复使用性。

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