College of Materials and Metallurgy, Wuhan University of Science and Technology, Wuhan, Hubei Province 430081, China.
J Colloid Interface Sci. 2013 Mar 15;394:166-76. doi: 10.1016/j.jcis.2012.11.059. Epub 2012 Dec 5.
Integration of 'green chemistry' principles into nanotechnology is one of the key issues in nanoscience research today. In this work, three series of Au/Pt bimetallic nanoparticles (BNPs) with a structure of Au-rich core/Pt-rich shell were prepared using simultaneous reduction with rapid injection of NaBH(4), simultaneous reduction with dropwise addition of NaBH(4), and simultaneous alcohol reduction. The effects of particle size, electronic structure and composition upon the catalytic activities for aerobic glucose oxidation of the BNPs were also investigated. Catalytically highly active PVP-protected Au/Pt BNPs of about 1.5 nm in diameter were synthesized using simultaneous reduction with rapid injection of NaBH(4). The prepared colloidal Au/Pt BNPs catalysts possessed a high and durable catalytic activity for aerobic glucose oxidation, which were stably kept for more than 2 months under ambient conditions. The maximum activities normalized with Au content of the BNPs with Au/Pt atomic ratio of 4/6 were nearly 10 times higher than that of Au nanoparticles (NPs) with nearly the same particle size. The higher catalytic activity of the prepared Au/Pt BNPs than the Au NPs can be ascribed to the following two factors; (1) the small average diameter, usually about 1.5 nm, and (2) the presence of negatively charged Au and Pt atoms due to electron donation from protecting polymer (PVP: poly(N-vinyl-2-pyrrolidone)) by electronic charge transfer effects upon catalytically active sites. In contrast, the Au/Pt BNPs, synthesized by alcohol reduction and dropwise addition of NaBH(4) into the starting solution and having the large mean particle sizes, showed a low catalytic activity.
将“绿色化学”原则融入纳米技术是当今纳米科学研究的关键问题之一。在这项工作中,使用 NaBH 4 快速注入同时还原、NaBH 4 逐滴添加同时还原和醇同时还原三种方法制备了具有富 Au 核/富 Pt 壳结构的 Au/Pt 双金属纳米粒子(BNPs)。还研究了粒径、电子结构和组成对 BNPs 有氧葡萄糖氧化催化活性的影响。使用 NaBH 4 快速注入同时还原法合成了约 1.5nm 直径的催化活性高的 PVP 保护的 Au/Pt BNPs。所制备的胶体 Au/Pt BNPs 催化剂对有氧葡萄糖氧化具有高且持久的催化活性,在环境条件下稳定保持 2 个月以上。具有 Au/Pt 原子比为 4/6 的 BNPs 的 Au 含量归一化的最大活性比具有几乎相同粒径的 Au 纳米粒子(NPs)高近 10 倍。与 Au NPs 相比,所制备的 Au/Pt BNPs 的更高催化活性可以归因于以下两个因素:(1)小的平均直径,通常约为 1.5nm,(2)由于电子转移效应,保护聚合物(PVP:聚(N-乙烯基-2-吡咯烷酮))向催化活性位点供电子,导致带负电荷的 Au 和 Pt 原子的存在。相比之下,通过将 NaBH 4 逐滴添加到起始溶液中并具有较大平均粒径的醇还原和 NaBH 4 同时还原合成的 Au/Pt BNPs 表现出低的催化活性。