Hairy Carbon Nanotube@Nano-Pd Heterostructures: Design, Characterization, and Application in Suzuki C-C Coupling Reaction
Hairy Carbon Nanotube@Nano-Pd Heterostructures: Design, Characterization, and Application in Suzuki C-C Coupling Reaction
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DOI：
10.1021/la102801d
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发表时间：
2010-10-19
期刊：
影响因子：
3.9
通讯作者：
Chehimi, Mohamed M.
中科院分区：
文献类型：
--
作者：
Chergui, Sarmia Mahouche;Ledebt, Alexandre;Chehimi, Mohamed M.
采用ATRP法在本体溶液中合成了聚甲基丙烯酸缩水甘油酯（PGMA），并对其环氧基进行了酸水解，得到了含甘油基团的聚合物（POH）。POH链端C-Br键受到NaN（3）的亲核攻击，产生叠氮封端的POH（POH-N（3））。碳纳米管通过从式H（2）N-C（6）H（4）-C C-H的对炔基化苯胺中原位生成的炔基化重氮阳离子进行修饰，产生CNT-C（6）H（4）-C-C-H纳米管。将叠氮化物官能化的聚合物POH-N（3）点击到炔基改性的CNT上，得到CNT@POH杂化物，将其进一步进行氧化，得到羧化的聚合物改性的CNT（记为CNT@PC00H）。所设计的毛状碳纳米管作为有效的平台，原位合成和大量负载的3 nm大小的钯纳米粒子（NPs）。到目前为止制备的CNT@ PCOOH@Pd异质结构在C-C Suzuki偶联反应中表现出有效的催化效果，并且再生多达四次而没有任何显着的催化活性损失。
Poly(glycidyl methacrylate), PGMA, was prepared via ATRP in bulk solution, and its epoxy groups were further acid-hydrolyzed in order to obtain a polymer with glycerol moieties (noted POH). The POH chain end C-Br bonds were subjected to a nucleophilic attack by NaN(3), resulting in azide-terminated POH (POH-N(3)). The CNTs were modified by in-situ-generated alkynylated diazonium cations from the para-alkynylated aniline of the formulas H(2)N-C(6)H(4)-C C-H, yielding CNT-C(6)H(4)-C- C-H nanotubes. The azide-functionalized polymer POH-N(3) was clicked to the alkynyl-modified CNTs giving CNT@POH hybrids, which were further subjected to an oxidation resulting in carboxylated polymer-modified CNTs (noted CNT@PCOOH). The as-designed hairy CNTs served as efficient platforms for the in-situ synthesis and massive loading of 3 nm sized palladium nanoparticles (NPs). The CNT@ PCOOH@Pd heterostructures prepared so far exhibited an efficient catalytic effect in the C-C Suzuki coupling reaction and were regenerated up to four times without any significant loss of catalytic activity.