Rapid Authentication of Plant-Based Milk Alternatives by Coupling Portable Raman Spectroscopy with Machine Learning.

Hieu M Le, Tianqi Li, Jimena G Villareal, Jie Gao, Yaxi Hu
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Abstract

Background: Plant-based milk alternatives (PBMA) are increasingly popular due to rising lactose intolerance and environmental concerns over traditional dairy products. However, limited efforts have been made to develop rapid authentication methods to verify their biological origin.

Objective: In this study, we developed a rapid, on-site analytical method for the authentication and identification of PBMA made by six different plant species utilizing a portable Raman spectrometer coupled with machine learning.

Methods: Unprocessed PBMA (i.e., blended raw nut/grain) and processed PBMA that mimic the industrial processing procedures (i.e., filtration and pasteurization) were prepared in lab and subjected to Raman spectral collection without any sample preparation. Three machine learning algorithms [i.e., k-nearest neighbor (KNN), support vector machine (SVM) and random forest (RF)] were tested and compared.

Results: RF achieved the best performance in recognizing the plant sources for the unprocessed PBMA, with accuracies of 96.88% and 95.83% in the cross-validation and test set prediction, respectively. Due to small sample size and risk of overfitting, classification models for the biological origin of processed PBMA were constructed by combining Raman spectra of the unprocessed and processed samples. Again, RF models achieved the highest accuracy in identifying the species, i.e., 94.27% in cross-validation and 94.44% in prediction.

Conclusions: These results indicated that the portable Raman spectrometer captured the chemical fingerprints that can effectively identify the plant species of different PBMA. Using this non-destructive Raman spectroscopic based method, the overall analysis from sample to answer was completed within 5 min, providing inspection laboratories a rapid and reliable screening tool to ensure the authenticity of the biological origin of PBMA.

Highlights: This study presents a novel method for rapid and non-destructive identification of the plant sources of PBMA (both unprocessed and processed) based on the Raman spectroscopic technique and machine learning algorithms.

便携式拉曼光谱与机器学习相结合的植物性牛奶替代品快速认证
背景:由于乳糖不耐症的增加和对传统乳制品的环境担忧,植物性牛奶替代品(PBMA)越来越受欢迎。然而,在开发快速认证方法以验证其生物来源方面所做的努力有限。目的:在本研究中,我们利用便携式拉曼光谱仪与机器学习相结合,开发了一种快速的现场分析方法,用于鉴定和鉴定六种不同植物种类的PBMA。方法:在实验室中制备未加工的PBMA(即混合生坚果/谷物)和模拟工业加工程序(即过滤和巴氏杀菌)的加工PBMA,并在没有任何样品制备的情况下进行拉曼光谱采集。测试和比较了三种机器学习算法[即k-最近邻(KNN),支持向量机(SVM)和随机森林(RF)]。结果:RF在识别未处理PBMA的植物来源方面表现最佳,交叉验证和测试集预测的准确率分别为96.88%和95.83%。由于样本量小,存在过拟合的风险,将未加工样品和加工样品的拉曼光谱相结合,构建了加工后PBMA的生物来源分类模型。同样,RF模型在物种识别方面取得了最高的准确率,即交叉验证准确率为94.27%,预测准确率为94.44%。结论:便携式拉曼光谱仪捕获的化学指纹图谱可有效鉴别不同PBMA的植物种类。采用这种基于非破坏性拉曼光谱的方法,从样品到答案的整体分析在5分钟内完成,为检测实验室提供了一种快速可靠的筛选工具,以确保PBMA生物来源的真实性。本研究提出了一种基于拉曼光谱技术和机器学习算法的快速无损鉴定PBMA植物来源(包括未加工和加工)的新方法。
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