Time-series characterization of various honey types under different storage conditions based on total polyphenol content and fluorescence properties

Takumi Murai , Teruki Tobari , Sota Kudo , Yoshito Saito
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Abstract

This study investigated fluorescence spectroscopy for evaluating honey quality changes during storage. Twenty-two honey varieties were stored at high (35 °C) and low (4 °C) temperatures for six months, with excitation-emission matrix (EEM) and total polyphenol content (TPC) measured every two months. Under high-temperature storage, TPC increased significantly while remaining stable at low-temperature. EEM measurements revealed five characteristic fluorescence peaks attributed to various compounds including amino acids, flavonoids, phenolic acids and Maillard reaction products. Using principal component scores obtained from principal component analysis (PCA) dimensionality reduction, support vector machine (SVM) classification achieved 81.82 % accuracy in distinguishing between early storage periods and late storage periods for high-temperature samples, while maintaining 59.09 % accuracy for low-temperature samples. Partial least squares regression (PLSR) models constructed using EEM data demonstrated robust TPC prediction capability with R²cv of 0.92, root mean square error cross validation (RMSECV) of 40.66 μg gallic acid equivalent/g and residual prediction deviation (RPD) of 3.61. Variable importance in projection (VIP) analysis indicated that fluorescence regions associated with flavonoids, phenolic acids and Maillard reaction products significantly contributed to TPC prediction. These findings demonstrate the potential of fluorescence spectroscopy as a non-destructive method for evaluating honey quality changes during storage, particularly under high-temperature conditions.

Abstract Image

基于总多酚含量和荧光性质的不同蜂蜜类型在不同储存条件下的时间序列表征
研究了荧光光谱法评价蜂蜜贮藏过程中品质变化的方法。22个蜂蜜品种在高(35°C)和低(4°C)温度下储存6个月,每两个月测量一次激发-发射矩阵(EEM)和总多酚含量(TPC)。高温贮藏时,TPC显著增加,低温贮藏时保持稳定。EEM测量显示了五个特征荧光峰,这些荧光峰属于不同的化合物,包括氨基酸、类黄酮、酚酸和美拉德反应产物。利用主成分分析(PCA)降维得到的主成分分数,支持向量机(SVM)分类在高温样品的早期和晚期储存期区分准确率达到81.82%,在低温样品的早期储存期和晚期储存期区分准确率为59.09%。利用EEM数据构建的偏最小二乘回归(PLSR)模型具有较强的TPC预测能力,R²cv为0.92,均方根误差交叉验证(RMSECV)为40.66 μg没食子酸等效/g,剩余预测偏差(RPD)为3.61。可变重要性投影(VIP)分析表明,与黄酮类化合物、酚酸和美拉德反应产物相关的荧光区域对TPC预测有显著贡献。这些发现证明了荧光光谱作为一种非破坏性的方法来评估蜂蜜在储存过程中的质量变化的潜力,特别是在高温条件下。
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