Quartz Crystal Microbalance Sensor Using Molecularly Imprinted Polymer For Histamine Determination

Histamine (HA) is a kind of biogenic amine widely existed in the food, especially aquatic product and fermented food. Consuming excess HA will lead to a series of allergic reactions and even death. In recent years, food poisoning caused by HA in spoiled food has occurred frequently. Therefore, it is necessary to establish a rapid, sensitive, highly selective method for histamine detection in food.In this study, a novel imprinted material using HA as template molecule,3-mercaptopropyltriethoxysilane (MPTES) as functional polymer, tetraethoxysilane (TEOS) as cross-linker according to optimization for histamine recognition was synthesized in sol-gel process. The adsorption performance of the prepared material was evaluated by adsorption equilibrium binding experiment and adsorption kinetics experiment, the result demonstrating a high mass transfer velocity and saturated adsorption capacity of the developed material.The developed material was used as sensitive membrane and immobilized on the surface of quartz crystal platinum electrode to fabricate a molecular imprinted quartz crystal sensor for histamine detection. Through the evaluation based on frequency change, the developed sensor exhibited a lower detection limit of7.49×10-4mg kg-1(S/N=3), wider concentration linear range from0.11×10-2mg L-1-4.45×10-2mg L-1and higher selectivity for histamine (selectivity coefficient>4.0) compared with similar molecules, good reproducibility and long-term stability.The developed sensor was applied to determine histamine in six different fish products and the traditional high-performance liquid chromatography (HPLC) method was used as validation. The accuracy and stability of the developed method was demonstrated by the satisfactory recoveries ranging from93.2%to101.6%with R.S.D from0.2%to4.3%. In addition, the histamine detected by the developed senor was great relative (correlation coefficient,0.9965) to the result of HPLC method signifying the precision of the developed method in practical application of histamine determination.