Journal of Molecular Liquids ( IF 5.3 ) Pub Date : 2020-08-22 , DOI: 10.1016/j.molliq.2020.114119 Luana Z. Silva , Marcos R. Mauricio , Pedro G. Dubiela , Alessandro F. Martins , Adley F. Rubira
Polymers containing amine moieties reduce Au(III) and stabilize gold nanoparticles (AuNPs). Such polymers can be used to synthesize AuNPs with controlled sizes and shapes, providing high stability to the colloidal solutions. A star amino-functionalized poly(glycidyl methacrylate) (PGMA) can quickly be prepared by epoxide ring-opening reactions. We functionalized the β-cyclodextrin-(PGMA)7 with diethanolamine (DEA) to create a star polymer (β-CD-(PGDEA)7) by atom transfer radical polymerization (ATRP), using β-cyclodextrin (β-CD) as macroinitiator. We determined the tertiary amine content (-NR2 = 0.63 mmol/g; R = -CH2-CH2-OH) on the star polymer by gravimetric analysis. The material β-CD-(PGDEA)7 reduces Au(III) and stabilize AuNPs, following a strategy in-situ. AuNPs (7.8 nm) were created by controlling the tertiary amine content/Au(III) molar ratio. The ratio 5 at pH 5.2 supports protonated -NR2H+ (that binds [AuCl4]−) and -NR2 (that stabilize AuNPs) on the star polymer structure, providing colloidal stability over 70 days at room temperature due to the high Zeta potential (+30 mV). The catalytic activity of the colloidal suspension containing the star polymer-capped AuNPs was investigated in the conversion of 4-nitrophenol to 4-aminophenol, using sodium borohydride as a hydrogen donor agent. A high catalyst activity (knor = 65.11 L/min μmol) was obtained at 0.0043 μmol/L AuNPs. The result is assigned to the excellent AuNPs stability imparted by star polymer coatings, showing that the star polymer does not influence the catalytic activity of the covered AuNPs.
中文翻译:
具有催化活性的星形氨基官能化聚甲基丙烯酸甘油酯稳定的金纳米颗粒复合材料,可还原4-硝基苯酚
含胺部分的聚合物可还原Au(III)并稳定金纳米颗粒(AuNPs)。此类聚合物可用于合成具有受控大小和形状的AuNP,从而为胶体溶液提供高稳定性。星形氨基官能化的聚(甲基丙烯酸缩水甘油酯)(PGMA)可以通过环氧化物开环反应快速制备。我们使用二乙醇胺(DEA)对β-环糊精(PGMA)7进行功能化,以原子转移自由基聚合(ATRP)的形式使用β-环糊精(β-CD)作为星形聚合物(β-CD-(PGDEA)7)。宏观引发剂。通过重量分析,我们确定了星形聚合物上的叔胺含量(-NR 2 = 0.63 mmol / g; R = -CH 2 -CH 2 -OH)。材料β-CD-(PGDEA)7按照原位策略还原Au(III)并稳定AuNPs 。通过控制叔胺含量/ Au(III)摩尔比可生成AuNP(7.8 nm)。pH 5.2时的比例5支持星形聚合物结构上的质子化-NR 2 H +(与[AuCl 4 ] -结合)和-NR 2(使AuNPs稳定),由于室温下的高胶态稳定性,在室温下可提供70天以上的胶体稳定性。 Zeta电位(+30 mV)。使用硼氢化钠作为氢供体,研究了由星形聚合物封端的AuNPs组成的胶体悬浮液在4-硝基苯酚向4-氨基苯酚的转化中的催化活性。高的催化剂活性(K也不 在0.0043μmol/ L的AuNP下获得= 65.11 L / minμmol)。结果归因于星形聚合物涂层赋予的优异的AuNPs稳定性,表明星形聚合物不会影响被覆AuNPs的催化活性。