本文選題：溫敏聚合物　切入點(diǎn)：金納米粒子　出處：《魯東大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：本論文通過異丁酸酐與超支化聚乙烯亞胺的胺基反應(yīng)制備了具有溫敏特性的異丁�；Щ垡蚁﹣啺�(HPEI-IBAm)。以具有大量胺基的HPEI-IBAm為還原劑,可將氯金酸還原制備出穩(wěn)定的金納米粒子。這種通過HPEI-IBAm與氯金酸原位還原反應(yīng)制備AuNPs的方法不需要另外加入小分子毒性還原劑,綠色環(huán)保,具有重要意義�；贖PEI-IBAm穩(wěn)定的金納米粒子(AuNPs)不僅可實(shí)現(xiàn)對銀離子的比色傳感檢測,還能實(shí)現(xiàn)對檢測后的AuNPs/銀復(fù)合物的分離。其比色檢測的機(jī)理為HPEI-IBAm可將銀離子還原成單質(zhì)銀,單質(zhì)銀吸附在AuNPs(紅色)表面,形成核殼金-銀納米粒子(棕色)。HPEI-IBAm具有很高的空間位阻效應(yīng),不僅可以穩(wěn)定金納米粒子,而且還可以為金-銀核殼納米粒子提供很好的穩(wěn)定作用,能夠使其長時間穩(wěn)定存在而不聚集,便于在顏色變化后對其進(jìn)行觀察和記錄。這種基于形成穩(wěn)定金-銀核殼納米粒子伴隨出現(xiàn)紅色到棕色獨(dú)特變化的比色傳感相比傳統(tǒng)的因AuNPs聚集引起紅到紫色(或藍(lán)色)變化的傳感器具有更高的選擇性。因?yàn)橹T如在酸度、溫度過高或固體狀態(tài)存在時都會引起傳統(tǒng)AuNPs聚集伴隨紅到紫色的顏色變化,干擾檢測結(jié)果的準(zhǔn)確性。并且聚集態(tài)的金納米粒子是不穩(wěn)定的,因此變化后的顏色不能長時間保持,不利于觀察記錄。整個檢測反應(yīng)過程迅速,大約在0.5-1分鐘左右就可以達(dá)到穩(wěn)定的顏色變化狀態(tài)。同時,該比色傳感器對銀離子的比色檢測具有高的靈敏度,其肉眼可分辨的檢測限為5.73?(44),紫外可見光譜檢測限為5.73 nM(遠(yuǎn)低于美國環(huán)境保護(hù)署制定的飲用水中銀離子的最高含量標(biāo)準(zhǔn)0.1 mg/L≈920 nM)。這種基于聚合物穩(wěn)定的金納米粒子對銀離子的檢測,相比小分子還原法制備金納米粒子的傳統(tǒng)比色傳感檢測具有更多的優(yōu)勢:(1)溫敏聚合物不僅可以作為綠色的還原劑和穩(wěn)定劑,把銀離子還原為零價的銀納米粒子,然后沉積在金納米粒子的表面,使得體系有很明顯的顏色變化,而且也是很好的分離劑,在檢測后可以利用其溫敏特性,把傳感器和銀的混合物分離出來。(2)聚合物穩(wěn)定的金納米粒子可以實(shí)現(xiàn)制備、檢測和分離的一體化,有利于節(jié)約能源、保護(hù)環(huán)境和實(shí)現(xiàn)可持續(xù)發(fā)展,并且為以后開發(fā)多功能納米復(fù)合材料提供了很好的思路。(3)這種聚合物制備的金納米粒子的穩(wěn)定性(即使在高溫、酸性介質(zhì)、固體粉末和高離子強(qiáng)度下)高,主要得益于聚合物末端有大量的胺基基團(tuán)和高的空間位阻效應(yīng),可以有效的避免酸性介質(zhì)和高離子強(qiáng)度的干擾以提高檢測銀離子的選擇性和唯一性。(4)這種金納米粒子比色檢測的顏色變化是由紅色到棕色的顏色變化,而且這種紅色到棕色的顏色變化是唯一的,可以通過眼睛觀察,展示了檢測體系的高靈敏度和對銀離子的高選擇性,(5)檢測后基于聚合物的溫敏特性,通過簡單的加熱沉淀或離心可實(shí)現(xiàn)AuNPs/Ag復(fù)合物的分離,可避免二次污染。
[Abstract]:In this paper, the iso-butyloyl hyperbranched polyimide (HPEI-IBAmN) was prepared by the reaction of isobutyric anhydride with the amine group of hyperbranched polyimine. HPEI-IBAm with a large number of amino groups was used as reducing agent. Stable gold nanoparticles can be prepared by reduction of chlorauric acid to prepare AuNPs by in-situ reduction reaction of HPEI-IBAm with chlorauric acid, which does not require the addition of small molecular toxic reductants, which is green and environmentally friendly. The au nanoparticles based on HPEI-IBAm can not only detect the silver ions, but also separate the silver complexes of AuNPs/. The mechanism of the colorimetric detection is that the silver ions can be reduced to silver by HPEI-IBAm. The adsorbed silver on the surface of AuNPs (red) forms a core-shell gold-silver nanoparticles (brown. HPEI-IBAm) with a high steric resistance effect, which can not only stabilize the gold nanoparticles, but also provide a good stability for the gold-silver core-shell nanoparticles. Can keep it stable for a long time without gathering, This colorimetric sensor based on the formation of stable gold-silver core-shell nanoparticles with unique red to brown variations is easier to observe and record when the color changes occur compared to the traditional red-purple resulting from AuNPs aggregation (or. Blue) changes in the sensor have higher selectivity because, for example, in acidity, When the temperature is too high or the solid state exists, the traditional AuNPs aggregation will be accompanied by the color change from red to purple, which will interfere with the accuracy of the detection results. Moreover, the gold nanoparticles in the aggregated state are unstable, so the color after the change cannot be maintained for a long time. It is not good for observation record. The whole process of detection reaction is rapid, and can reach a stable color change state in about 0.5-1 minute. At the same time, the colorimetric sensor has high sensitivity to the colorimetric detection of silver ions. The detectable limit of its naked eye is 5.73? The UV / Vis detection limit is 5.73 nm (which is far below the US Environmental Protection Agency's highest standard for silver ions in drinking water: 0.1 mg/L 鈮，

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