Aroma is an important factor in evaluating tea infusion quality. In this study, the aroma quality of 44 Dianhong Congou tea infusions was classified into high-quality group and non-high-quality group according to the sensory evaluation. The volatile components were investigated by using headspace solid phase microextraction combined with comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry. A total of 258 volatile components were identified, of which the three component types with the highest relative percentages were alcohols (17.05%), aldehydes (15.12%), and heterocycles (15.12%). Clear discrimination was achieved by orthogonal partial least squares discrimination analysis (R2Y = 0.94, Q2 = 0.82). In addition, 69 important differential compounds were identified based on variable importance in the projection value (VIP >1.0) and one-way ANOVA (p < 0.05). Moreover, seven common key odorants with odor activity values (OAVs) > 1 were screened out, including (E, E)-2,4-heptadienal, linalool, 1-octene-3-one, geraniol, β-myrcene, (Z)-4-heptenal, and nonanal. Aroma character impact value indicated that linalool performed a positively supportive role in the aroma quality of Dianhong Congou tea infusions, while (E, E)-2,4-heptadienal negatively affected the aroma quality. These results contribute to providing a theoretical support for directional processing of high-quality black tea.
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