Liu Mengxiao, Zhang Hongli, Shu Jiangnan, Liu Xiaoyang, Li Fang, Cui Hua
CAS Key Laboratory of Soft Matter Chemistry, Department of Chemistry, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
Anal Chem. 2014 Mar 18;86(6):2857-61. doi: 10.1021/ac5002433. Epub 2014 Mar 4.
Despite much progress in functionalized gold nanomaterial (GNMs), chemiluminescent (CL) functionalized GNMs with high CL efficiency are far from fully developed. In this work, we report a general strategy for the synthesis of gold nanoparticles (GNPs) bifunctionalized by CL reagent and catalyst metal complexes (BF-GNPs) by taking N-(aminobutyl)-N-(ethylisoluminol) (ABEI) as a model of CL reagents. The complexes of 2-[bis[2-[carboxymethyl-[2-oxo-2-(2-sulfanylethylamino)ethyl]amino]ethyl]amino]acetic acid (DTDTPA) with various metal ions, including Co(2+), Cu(2+), Pb(2+), Ni(2+), Hg(2+), Cr(3+), Eu(3+), La(3+), Gd(3+), Sm(3+), Er(3+), Dy(3+), Ce(4+), and Ce(3+), were grafted on the surface of ABEI functionalized GNPs (ABEI-GNPs) to form a series of BF-GNPs. These BF-GNPs exhibited excellent CL activity. In particular, the CL intensity of DTDTPA/Co(2+)-ABEI-GNPs was over 3 orders of magnitude higher than ABEI-GNPs. This work demonstrates for the first time that metal complexes grafted on the surface of GNPs have unique catalytic activity on the CL reaction, superior to that in the liquid phase. Such BF-GNPs may find future applications in bioassays, microchips, and molecular/cellular imaging.
尽管功能化金纳米材料（GNMs）取得了很大进展，但具有高化学发光（CL）效率的化学发光功能化GNMs仍远未得到充分发展。在这项工作中，我们报告了一种以N-(氨丁基)-N-(乙基异鲁米诺)（ABEI）作为化学发光试剂模型，合成由化学发光试剂和催化金属配合物双功能化的金纳米颗粒（BF-GNPs）的通用策略。2-[双[2-[羧甲基-[2-氧代-2-(2-巯基乙氨基)乙基]氨基]乙基]氨基]乙酸（DTDTPA）与包括Co(2+)、Cu(2+)、Pb(2+)、Ni(2+)、Hg(2+)、Cr(3+)、Eu(3+)、La(3+)、Gd(3+)、Sm(3+)、Er(3+)、Dy(3+)、Ce(4+)和Ce(3+)在内的各种金属离子形成的配合物被接枝到ABEI功能化的GNPs（ABEI-GNPs）表面，形成了一系列BF-GNPs。这些BF-GNPs表现出优异的化学发光活性。特别是，DTDTPA/Co(2+)-ABEI-GNPs的化学发光强度比ABEI-GNPs高出3个数量级以上。这项工作首次证明了接枝在GNPs表面的金属配合物对化学发光反应具有独特的催化活性，优于液相中的催化活性。这种BF-GNPs未来可能在生物测定、微芯片和分子/细胞成像中得到应用。
