Abstract
Organic acids have essential effects on the flavor of Baijiu. Except for some small molecular organic acids, which are volatile, most of other organic acids are non-volatile. And due to their low contents in Baijiu, the detection of non-volatile organic acids (NVOAs) in Baijiu is a challenging work. In this study, an optimized derivatization method was developed to detect the NVOAs in Baijiu. Optimization on the derivatization reagent, reaction time and temperature revealed that 10 mL of Baijiu was concentrated to dryness, followed by adding 100 μL BSTFA and 50 μL pyridine and subsequent derivatization over 3 h at 80 °C was suitable. Under the optimal conditions, excellent linearity for all NVOAs was obtained with determination coefficients of R2 > 0.99, inter-day and intra-day precision were below 7.30% and 6.90%, respectively, and recovery rates were in the range of 80.64–113.46%. The LODs were between 0.05 and 11.75 μg/L, which were one-fifth to one ten-thousandth of those detected by HPLC and HPLC–MS. Thirty-six NVOAs in soy sauce (SS), strong (ST), and Laobaigan (LBG) flavor-types of Baijiu were identified. The concentration of lactic acid among the three types of Baijiu was the highest, whose contents were (1069.16 ± 58.74, 7330.11 ± 47.67, 2054.02 ± 54.15) mg/L in LBG, SS, and ST, respectively. Besides, the NVOAs in these three Baijiu were quite different according to principal component analysis and hierarchical cluster analysis. This study provides an effective method for the analysis of NVOAs in complex matrix foods.
Similar content being viewed by others
Data Availability
Not applicable.
Code Availability
Not applicable.
References
Deng N, Du H, Xu Y (2020) Cooperative response of pichia kudriavzevii and saccharomyces cerevisiae to lactic acid stress in Baijiu fermentation. J Agric Food Chem 68(17):4903–4911. https://doi.org/10.1021/acs.jafc.9b08052
Fan W, Qian MC (2006) Characterization of aroma compounds of Chinese “wuliangye” and “jiannanchun” liquors by aroma extract dilution analysis. J Agric Food Chem 54(7):2695–2704. https://doi.org/10.1021/jf052635t
Ferreira V, Jarauta I, López R, Cacho J (2003) Quantitative determination of sotolon, maltol and free furaneol in wine by solid-phase extraction and gas chromatography-ion-trap mass spectrometry. J Chromatogr A 1010(1):95–103. https://doi.org/10.1016/S0021-9673(03)00963-4
Frank S, Wollmann N, Schieberle P, Hofmann T (2011) Reconstitution of the flavour signature of dornfelder red wine on the basis of the natural concentrations of its key aroma and taste compounds. J Agric Food Chem 59(16):8866–8874. https://doi.org/10.1021/jf202169h
Gracia-Moreno E, Lopez R, Ferreira V (2015) Quantitative determination of five hydroxy acids, precursors of relevant wine aroma compounds in wine and other alcoholic beverages. Anal Bioanal Chem 407(26):7925–7934. https://doi.org/10.1007/s00216-015-8959-9
Haas M, Lamour S, Trapp O (2018) Development of an advanced derivatization protocol for the unambiguous identification of monosaccharides in complex mixtures by gas and liquid chromatography. J Chromatogr A 1568:160–167. https://doi.org/10.1016/j.chroma.2018.07.015
Halket JM, Zaikin VG (2003) Derivatization in mass spectrometry-1 silylation. Eur J Mass Spectrom 9(1):1–21. https://doi.org/10.1255/ejms.527
Hofmann T, Krautwurst D, Schieberle P (2018) Current status and future perspectives in flavour research: highlights of the 11th wartburg symposium on flavour chemistry & biology. J Agric Food Chem 66(10):2197–2203. https://doi.org/10.1021/acs.jafc.7b06144
Hofstetter CK, Dunkel A, Hofmann T (2019) Unified flavour quantitation: toward high-throughput analysis of key food odorants and tastants by means of ultra-high-performance liquid chromatography tandem mass spectrometry. J Agric Food Chem 67(31):8599–8608. https://doi.org/10.1021/acs.jafc.9b03466
Ivanova-Petropulos V, Tašev K, & Stefova M (2016) HPLC method validation and application for organic acid analysis in wine after solid-phase extraction. Maced J Chem Chem En 35(2):225–233. https://doi.org/10.20450/mjcce.2016.1073
Jia W, Fan Z, Du A, Li Y, Zhang R, Shi Q, Shi L, Chu X (2020) Recent advances in Baijiu analysis by chromatography based technology-a review. Food Chem 324:126899. https://doi.org/10.1016/j.foodchem.2020.126899
Jin G, Zhu Y, Xu Y (2017) Mystery behind Chinese liquor fermentation. Trends Food Sci Technol 63:18–28. https://doi.org/10.1016/j.tifs.2017.02.016
Li J, Shui Z, Dong L, Shen L, Zhao D, Luo H, Ma Y, Hou C, Huo D (2020) A novel acid-sensitive quantum dot sensor array for the identification of Chinese Baijiu. Anal Methods 12(39):4789–4797. https://doi.org/10.1039/d0ay01454k
Liao Q, Lian S, Li Y, Li Q (2013) Determination of higher fatty acids in liquor by LC-QTOF. Liquor-Making Sci & Tech 10:97–99
Liu H, Sun B (2018) Effect of fermentation processing on the flavour of Baijiu. J Agric Food Chem 66(22):5425–5432. https://doi.org/10.1021/acs.jafc.8b00692
Mato I, Suárez-Luque S, Huidobro JF (2005) A review of the analytical methods to determine organic acids in grape juices and wines. Food Res Int 38(10):1175–1188. https://doi.org/10.1016/j.foodres.2005.04.007
McGovern PE, Zhang J, Tang J, Zhang Z, Hall GR, Moreau RA, Nunez A, Butrym ED, Richards MP, Wang CS, Cheng G, Zhao Z, Wang C (2004) Fermented beverages of pre- and proto-historic China. Proc Nat Acad Sci USA 101(51):17593–17598. https://doi.org/10.1073/pnas.0407921102
Medeiros PM, Simoneit BRT (2007) Analysis of sugarsin environmental samples by gas chromatography-mass spectrometry. J Chromatogr A 1141(2):271–278. https://doi.org/10.1016/j.chroma.2006.12.017
Regueiro J, Negreira N, Simal-Gandara J (2017) Challenges in relating concentrations of aromas and tastes with flavour features of foods. Crit Rev Food Sci Nutr 57(10):2112–2127. https://doi.org/10.1080/10408398.2015.1048775
Sáenz-Navajas M, Campo E, Culleré L, Fernández-Zurbano P, Valentin D, & Ferreira V (2010) Effects of the nonvolatile matrix on the aroma perception of wine. J Agric Food Chem 58(9):5574-5585. https://doi.org/10.1021/jf904377p
Schummer C, Delhomme O, Appenzeller B, Wennig R, Millet M (2009) Comparison of MTBSTFA and BSTFA in derivatization reactions of polar compounds prior to GC/MS analysis. Talanta 77(4):1473–1482. https://doi.org/10.1016/j.talanta.2008.09.043
Shareef A, Angove MJ, Wells JD (2006) Optimization of silylation using N-methyl-N-(trimethylsilyl)-trifluoroacetamide, N, O-bis-(trimethylsilyl)-trifluoroacetamide and N-(tert-butyldimethylsilyl)-N-methyltrifluoroacetamide for the determination of the estrogens estrone and 17α-ethinylestradiol by gas chromatography-mass spectrometry. J Chromatogr A 1108(1):121–128. https://doi.org/10.1016/j.chroma.2005.12.098
Song W, Lizhaojie Y, Wangkai G, Lilinjie, & Jiangweizhen, (2017a) Rapid determination of various organic acids and anions in Baijiu by ion chromatography. China Brewing 36(11):153–157
Song X, Wang G, Zhu L, Ji J, Zheng F, Sun J, Li H, Huang M, Zhao Q, Zhao M, Sun B (2021) Comparison of two cooked vegetable aroma compounds, dimethyl disulfide and methional, in Chinese Baijiu by a sensory-guided approach and chemometrics. LWT Food Sci Technol 2021:111427. https://doi.org/10.1016/j.lwt.2021.111427
Song X, Jing S, Zhu L, Ma C, Song T, Wu J, Zhao Q, Zheng F, Zhao M, Chen F (2020) Untargeted and targeted metabolomics strategy for the classification of strong aroma-type Baijiu (liquor) according to geographical origin using comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry. Food Chem 314:126098. https://doi.org/10.1016/j.foodchem.2019.126098
Song X, Zhu L, Wang X, Zheng F, Zhao M, Liu Y, Li H, Zhang F, Zhang Y, Chen F (2019) Characterization of key aroma-active sulfur-containing compounds in Chinese laobaigan Baijiu by gas chromatography-olfactometry and comprehensive two-dimensional gas chromatography coupled with sulfur chemiluminescence detection. Food Chem 297:124959. https://doi.org/10.1016/j.foodchem.2019.124959
Song Z, Du H, Zhang Y, Xu Y (2017b) Unraveling core functional microbiota in traditional solid-state fermentation by high-throughput amplicons and metatranscriptomics sequencing. Front Microbiol 8. https://doi.org/10.3389/fmicb.2017.01294
Xiang L, Zhu L, Huang Y, Cai Z (2020) Application of derivatization in fatty acids and fatty acyls detection: mass spectrometry-based targeted lipidomics. Small Methods 4(8):2000160. https://doi.org/10.1002/smtd.202000160
Yang H, Fan W, Xu Y (2017) Characterization of non-volatile organic acids in Baijius (Chinese liquors) based on BSTFA derivatization coupled with GC-MS. Food Ferment Ind 43(5):192–197
Zhang J, Tian Z, Ma Y, Shao F, Huang J, Wu H, Tian L (2019) Origin identification of the sauce-flavour Chinese Baijiu by organic acids, trace elements, and the stable carbon isotope ratio. J Food Quality 2019:1–7. https://doi.org/10.1155/2019/7525201
Zhang X, Wang C, Wang L, Chen S, Xu Y (2020) Optimization and validation of a head space solid-phase microextraction-arrow gas chromatography-mass spectrometry method using central composite design for determination of aroma compounds in Chinese liquor (Baijiu). J Chromatogr A 1610:460584. https://doi.org/10.1016/j.chroma.2019.460584
Zheng F, Ma Y, Hou M, Sun J, Sun X, Huang M, Li H, Sun B (2017) Progress and prospect in aroma components in top six distilled spirits. J Food Sci and Tech 35(2):1–12
Zheng X, Han B (2016) Baijiu (白酒), Chinese liquor: history, classification and manufacture. J Ethnic Foods 3(1):19–25. https://doi.org/10.1016/j.jef.2016.03.001
Funding
This work was supported by the National Key R&D Program of China [2016YFD0400500] and the National Natural Science Foundation of China [32001826].
Author information
Authors and Affiliations
Contributions
Guangnan Wang: investigation and writing-original draft. Xing Li: data curation and investigation. Xuebo Song: investigation and software. Si Jing: investigation and software. Shihao Meng: software. Fuping Zheng: research scheme design and supervision. Hehe Li: software. Zexia Li: supervision. Caihong Shen: supervision. Yi Shen: supervision.
Corresponding author
Ethics declarations
Ethics approval
This article does not contain any results from studies involving human participants or animals performed by any of the authors.
Consent to Participate
Not applicable.
Consent for Publication
Not applicable.
Conflict of Interest
Guangnan Wang declares that he/she has no Conflict of interest. Xing Li declares that he/she has no Conflict of interest. Xuebo Song declares that he/she has no Conflict of interest. Si Jing declares that he/she has no Conflict of interest. Shihao Meng declares that he/she has no Conflict of interest. Fuping Zheng declares that he/she has no Conflict of interest. Hehe Li declares that he/she has no Conflict of interest. Zexia Li declares that he/she has no Conflict of interest. Caihong Shen declares that he/she has no Conflict of interest. Yi Shen declares that he/she has no Conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Wang, G., Li, X., Song, X. et al. Optimization and Validation of a Method for Analysis of Non-Volatile Organic Acids in Baijiu by Derivatization and its Application in Three Flavor-Types of Baijiu. Food Anal. Methods 15, 1606–1618 (2022). https://doi.org/10.1007/s12161-021-02215-w
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s12161-021-02215-w