金/二硫化鉬/硫摻雜石墨烯量子點之類過氧化酶活性快速檢測2-硫醇苯駢塞唑研究

Peroxidase-Like Activity of Au/MoS2/SGQDs for Rapid Detection of 2-Mercaptobenzothiazole in Water Environment

王翊庭(Yi-Ting. Wang)

指導教授 ： 董瑞安

國立清華大學/原子科學院/生醫工程與環境科學系/碩士(2020年)

摘要

高度的工業發展與科技的進步，衍生出許多環境污染的問題，存在於水環境中的致癌物質比比皆是，近年來，為了改善以往使用液相層析儀檢測之昂貴、耗時與廢液等問題，生物(Biosensor)及化學感測器(Chemical Sensor)的研究推陳出新。故本研究期望開發一簡單、經濟、快速兼具高靈敏度與選擇性之方法，檢測由國際癌症研究中心(IARC)列為Group 2A級之致癌物2-硫醇苯駢塞唑(MBT)，其主要來自橡膠製品製造所需硫化促進劑與工業用抗腐蝕劑。本研究成功複合過渡金屬二硫化物(TMD)的奈米片狀二硫化鉬(MoS2)與硫摻雜石墨烯量子點(SGQDs)形成MoS2/SGQDs，並修飾奈米金粒子(Au nanoparticles)於表面上，製備出Au/MoS2/SGQDs，作為一新型的奈米酶材料，並利用其類過氧化酶之活性催化過氧化氫(H2O2)與3,3',5,5'-四甲基聯苯胺(TMB)所組成的系統，透過Au/MoS2/SGQDs之間MBT化學鍵的生成，影響催化之活性並有效地檢測水中MBT濃度；結果顯示，本開發之系統對MBT的感測濃度範圍為10 nM至1200 nM，R2值高達0.994，最低偵測極限(LOD)可達0.3324 nM，低於US EPA之規範值約100倍。此外，Au/MoS2/SGQDs對MBT具有很高的選擇性，不受複雜基質存在下影響表現，已成功應用於自來水、河水與埤塘水樣，其回收率在90±2 %至113±5%之間，為未來對於檢測低濃度而高毒性的環境致癌因子MBT提供一具有發展潛力之分析方向。

關鍵字

二硫化鉬 ； 石墨烯量子點 ； 奈米金粒子 ； 奈米酶 ； 類過氧化酶 ； 2-硫醇苯駢塞唑

並列摘要

Rapid industrial and technological development entails many environmental issues including the presence of carcinogens in the water environment. A number of research have been conducted focusing on the detection of these pollutants as key to solving these environmental problems. However, most of these technologies are costly, time consuming and produces waste liquid from the detection system such as high performance liquid chromatography detection. Due to this, research on biosensor and chemical sensor were innovated having advantages such as relatively cheap, fast detection mechanism and avoid the production of waste liquid.
In this study, we expect to develop a simple, economical and rapid method with high sensitivity and selectivity to detect 2-Mercaptobenzothiazole (MBT), which is classified as Group 2A carcinogens level by the International Cancer Research Center (IARC). The combination of molybdenum disulfide nanosheet (MoS2) from transition metal disulfide (TMD) family, sulfur-doped graphene quantum dots (SGQDs), and modified Au nanoparticles on the surface, forming Au/MoS2/SGQDs novel nanocomposite was successfully synthesized in this work. Au/MoS2/SGQDs were prepared as a new type of nanozyme material which uses its intrinsic peroxidase-like activity to catalyze the reaction between hydrogen peroxide (H2O2) and 3,3’,5,5’-tetramethylbenzidine (TMB).
Through the formation of Au-S bond between MBT and Au/MoS2/SGQDs, the catalytic activity was greatly influenced by the various concentration of MBT in solution. Under optimal conditions, the results show that the concentration range of MBT detection in this system is from 10 nM to 1200 nM having R2 value of 0.994, and the lowest detection limit (LOD) can reach up to 0.3324 nM, which is about 100 times lower than the US EPA regulation. In addition, Au/MoS2/SGQDs exhibits high selectivity toward MBT detection over 19 other interferences. It has also been successfully applied to tap water, river water and pond water with a recovery in the range of 90±2 to 113±5 %. This sensing system can serve as a new avenue for sensor system in the effective detection of carcinogens in the water environment.

並列關鍵字

Molybdenum disulfide ； Graphene quantum dots ； Gold nanoparticle ； Nanozyme ； Peroxidase-like ； 2-Mercaptobenzothiazole

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