Synthesis and characterization of silica nanoparticles functionalized with multiple TEMPO groups and investigation on their oxidation activity
Synthesis and characterization of silica nanoparticles functionalized with multiple TEMPO groups and investigation on their oxidation activity
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多个TEMPO基团功能化二氧化硅纳米粒子的合成、表征及其氧化活性研究
DOI：
10.1039/c5py01190f
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发表时间：
2015-10
影响因子：
4.6
通讯作者：
Wang, Guowei
中科院分区：
文献类型：
--
作者：
Liu, Yujie;Wang, Xuepu;Song, Wenguang;Wang, Guowei
采用一种新颖、高效、通用的方法合成了一系列具有多个TEMPO基团的新型二氧化硅纳米粒子。首先，采用改进的APTES和TEOS试剂一锅法水解共缩合法制备了氨基功能化二氧化硅纳米粒子(SN-NH2)，并以2-溴异丁基溴为大分子引发剂，通过酰胺化反应对其进行了改性。然后，通过表面引发的原子转移自由基聚合(SI-ATRP)过程，控制地实现了具有致密的PGMA侧链壳层的聚合物接枝二氧化硅纳米颗粒(SN-g-PGMA)。随后，通过环氧化物与叠氮化钠试剂的定量开环反应，将叠氮基团引入到PGMA侧链上，并通过有效的与目标SN-g-(PGMA-TEMPO)的炔丙基-TEMPO的“点击”化学进一步连接TEMPO基团。红外光谱、电子顺磁共振、X射线光电子能谱、透射电子显微镜、核磁共振氢谱和热重分析表明目标聚合物和中间体的合成是成功的。作为一项重要的工作，对合成的SN-g-(PGMA-TEMPO)的催化活性进行了评价，并根据Anelli法考察了其对苯甲醇的氧化活性，同时也证实了该催化剂具有良好的催化效率、稳定性和可回收性。
A series of novel silica nanoparticles functionalized with multiple TEMPO groups were synthesized using a novel, efficient and versatile protocol. First, the amino-functionalized silica nanoparticles (SN-NH2) were obtained using an improved one-pot hydrolysis and co-condensation procedure of APTES and TEOS agents, and further modified with 2-bromoisobutyryl bromide for macro-initiator (SN-Br) by amidation reaction. Then, the polymer grafted silica nanoparticles (SN-g-PGMA) with a dense shell layer of PGMA side-chains were realized via the surface-initiated atom transfer radical polymerization (SI-ATRP) procedure in a controlled manner. Subsequently, the azido groups were introduced onto PGMA side-chains by the quantitative ring-opening reaction of an epoxide with a sodium azide agent, and the TEMPO groups were further attached by efficient “Click” chemistry with propargyl-TEMPO for the target SN-g-(PGMA-TEMPO). The evidence for the successful synthesis of target polymers and intermediates was sufficiently provided by FT-IR, EPR, XPS, TEM, 1H NMR, and TGA measurements. As an important task, the catalytic activity of the synthesized SN-g-(PGMA-TEMPO) was evaluated by the oxidation of benzylic alcohols according to the Anelli protocol, as well as the excellent efficiency, stability and recyclability of the catalyst were also confirmed.
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影响因子：
4.3
作者：
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通讯作者：
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影响因子：
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作者：
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影响因子：
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作者：
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通讯作者：
Wang, Guowei
影响因子：
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作者：
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通讯作者：
Zhmud, BV
影响因子：
5.5
作者：
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通讯作者：
A. Shaabani;E. Farhangi;Abbas Rahmati