合金纳米粒子的制备及其在重金属离子传感器构建中的应用研究

Nowadays the heavy metal pollution has become one of the major environmental problems. It is particularly urgent to establish and develop the simultaneous detection technology of heavy metal ions. The visual sensor arrays, which offer advantages in accuracy, simple and low cost for the simultaneous detection and discrimination of multiple analytes, have received increasing attention in recent years. Gold-metal nanoparticles are the ideal colorimetric sensor array materials due to their various colours depending on their sizes, shapes and interparticle distances. Therefore, the proposed project aims to simultaneously detect a variety of heavy metal ions through preparing pleochroic gold-metal nanoparticles and extracting the color-difference. The proposed method to greenly synthesize gold-metal nanoparticles is shown as following: addition of collagen to HAuCl4 solution, turns Au(III) to Au(I) anions, which are further mixed with low concentrations of heavy metal ions, and reduced by pepsin in the presence of luminol and H2O2, to form pleochroic gold-metal nanoparticles. By means of extracting the color difference, such as red, green and blue (RGB), a three-channel based colorimetric sensor array is fabricated to detect and discriminate heavy metal ions at low concentrations. The applicability of the proposed method would be verified by determination of ionized heavy metals in industrial waste water and haze. At the same time, we will apply molecular dynamics (MD) to simulate the reaction process and density functional theory (DFT) to calculate the property parameters of reactants and reaction products. The theoretical calculations would be compared with experimental measurements to explain the reaction mechanism.

重金属污染已成为当今主要环境问题之一。建立和发展同时检测多种重金属离子的分析技术显得尤为迫切。可视化阵列传感由于具有精确、简单、成本低等优点而获得更多青睐。合金纳米粒子的尺寸、形貌及聚集状态能够调控胶体颜色，是构建可视化阵列传感器的理想指示剂。因此本项目拟使用胶原蛋白酶，将Au(III)还原为Au(I)，将其与重金属离子混合，在此混合液中添加胃蛋白酶、鲁米诺和双氧水，通过调控实验条件，可控制备出不同形貌、大小的合金（金-重金属）纳米粒子。接着提取合金纳米粒子生成前后溶液的颜色，构建可视化阵列传感器，实现多种重金属离子的同时检测。随后应用发展的方法实现实际样品（工业废水和雾霾）中重金属离子检测。同时，采用分子动力学模拟实验反应过程和密度泛函理论计算反应物及反应产物的物性参数，结合实验测试数据，揭示反应机理。

重金属污染是现今突出的环境污染问题，绿色制备合金纳米粒子、基于其色差分析构建可视化阵列传感器，实现多种重金属离子的同时检测，并阐明反应机理，具有重要的科学意义。本项目使用绿色还原剂-蛋白质，还原三价金—Au(III)生成一价金—Au(I)，将其与较低浓度的重金属离子混合，调控实验条件，实现可控制备出不同形貌和不同大小的合金（金-重金属）纳米粒子。随后提取合金纳米粒子生产前后的溶液颜色—红、绿和蓝色，构建三通道可视化阵列传感器，实现多种重金属离子的同时检测。同时，本项目研究采用盐酸羟胺、硼氢化钠作为还原剂，实现不同尺寸、形貌纳米金的可控制备，利用纳米金独特的光学特性构造可视化阵列传感器。构建的传感器具有简单、快速、低成本和多组分同类物质同时区分与检测等优势。主要研究包括：1)精确调控还原剂的浓度、热力学和动力学等参数，实现纳米金和合金的可控制备；2) 采集并提取纳米金光学颜色，构建可视化阵列传感器，实现不同浓度多种同类物质（如重金属离子、蛋白质和抗生素）的同时检测，并考察传感器在实际样品中特定物质的分析检测应用。本项目研究有望拓展纳米金在可视化传感技术领域的应用前景。项目主持人以第一兼通讯作者身份发表SCI学术论文6篇，其中一篇学术论文（Yumin Leng*, et al. Langmuir, 2017, 33, 6398-6403）发表前后得到高分子化学创始人、1987年诺贝尔奖得主Jean-maire Lehn教授的支持！授权的中国发明专利4项。