牡丹皮药材熏硫及脱硫前后化学成分差异分析
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摘要
目的:本研究旨在分析熏硫及脱硫前后牡丹皮中化学成分的变化,为科学评价熏硫、脱硫牡丹皮的质量提供参考依据,为熏硫、脱硫对其他中药质量的影响的研究提供新的思路。方法:运用超高效液相-四极杆-线性离子阱质谱(UPLC-QTRAP-MS/MS)对正常、熏硫、脱硫牡丹皮中10种次生代谢产物的含量进行定量测定,分析熏硫、脱硫过程中化学成分的变化。同时运用《中华人民共和国药典》(2015年版)二氧化硫残留量测定法,测定了脱硫前后的熏硫牡丹皮中SO2残留量,对熏硫程度与牡丹皮中次生代谢产物的关系进行了分析。结果:牡丹皮熏硫后,苯甲酰芍药苷、苯甲酰氧化芍药苷及丹皮酚的含量显著降低(P<0.05);丹皮酚新苷及丹皮酚原苷的含量显著升高(P<0.05);芍药苷、五没食子酰葡萄糖苷、氧化芍药苷及没食子酸甲酯的含量有所升高,但两组没有显著性差异;没食子酸的含量变化不大。熏硫牡丹皮经脱硫处理后,除没食子酸、五没食子酰葡萄糖苷的含量显著降低以外,其他8种次生代谢产物的含量均不同程度地降低。结论:熏硫和脱硫过程均会导致牡丹皮中化学成分含量发生较大的变化,影响牡丹皮质量,因此,不建议在产地加工中使用熏硫和脱硫的加工方法。
Objective: To analyze the compounds difference in sulfured and desulfured Cortex Moutan Radicis, in order to provide references for scientific evaluation on the quality of sulfured and desulfured Cortex Moutan Radicis, and provide new idea for the quality research on sulfured and desulfured Chinese materia medica. Methods: Ten secondary metabolites in normal, sulfured and desulfured Cortex Moutan Radicis was determined based on UPLC-QTRAP-MS/MS and chemical compounds changes were analyzed. In the same time, residual SO2 was determined according to Chinese Pharmacopoeia, the relationship between sulfur fumigation degree and secondary metabolites in Cortex Moutan Radicis was analyzed. Results:Benzoyloxypaeoniflorin, benzoylpaeoniflorin and paeonol significantly reduced in sulfuring process(P<0.05), apiopaeonoside and paeonolide increased significantly in this process(P<0.05). Paeoniflorin, pentagaloyl glucoside, oxypaeoniflorin and methy gallate increased in sulfured Cortex Moutan Radicis, but there was no significant difference between two groups. There was no significant difference on the concentration of gallic acid. After desulfuring process, except for the decrease of gallic acid and pentagaloyl glucoside, the other 8 compounds decreased to different extent. Conclusion: Both sulfuring and desulfuring process can lead to great changes in the chemical composition of Cortex Moutan Radicis, and it would affect the quality of Cortex Moutan Radicis.So, it's not recommended to use sulfuring and desulfuring methods in the processing of Cortex Moutan Radicis.
Objective: To analyze the compounds difference in sulfured and desulfured Cortex Moutan Radicis, in order to provide references for scientific evaluation on the quality of sulfured and desulfured Cortex Moutan Radicis, and provide new idea for the quality research on sulfured and desulfured Chinese materia medica. Methods: Ten secondary metabolites in normal, sulfured and desulfured Cortex Moutan Radicis was determined based on UPLC-QTRAP-MS/MS and chemical compounds changes were analyzed. In the same time, residual SO2 was determined according to Chinese Pharmacopoeia, the relationship between sulfur fumigation degree and secondary metabolites in Cortex Moutan Radicis was analyzed. Results:Benzoyloxypaeoniflorin, benzoylpaeoniflorin and paeonol significantly reduced in sulfuring process(P<0.05), apiopaeonoside and paeonolide increased significantly in this process(P<0.05). Paeoniflorin, pentagaloyl glucoside, oxypaeoniflorin and methy gallate increased in sulfured Cortex Moutan Radicis, but there was no significant difference between two groups. There was no significant difference on the concentration of gallic acid. After desulfuring process, except for the decrease of gallic acid and pentagaloyl glucoside, the other 8 compounds decreased to different extent. Conclusion: Both sulfuring and desulfuring process can lead to great changes in the chemical composition of Cortex Moutan Radicis, and it would affect the quality of Cortex Moutan Radicis.So, it's not recommended to use sulfuring and desulfuring methods in the processing of Cortex Moutan Radicis.
引文
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[14]王巧,郭洪祝,霍长虹,等.白芍加工产物芍药苷亚硫酸酯的提取分离和结构鉴定.“以岭医药杯”全国青年药学工作者最新科研成果交流会论文集,2006
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[3]国家药典委员会.中华人民共和国药典.一部.北京:中国医药科技出版社,2015
[4]Wang X H,Xie P S,Lam C W,et al.Study of the destructive effect to inherent quality of Angelicae dahuricae radix(Baizhi)by sulfur-fumigated process using chromatographic fingerprinting analysis.Journal of Pharmaceutical&Biomedical Analysis,2009,49(5):1221-1225
[5]Li S L,Shen H,Zhu L Y,et al.Ultra-high-performance liquid chromatography-quadrupole/time of flight mass spectrometry based chemical profiling approach to rapidly reveal chemical transformation of sulfur-fumigated medicinal herbs,a case study on white ginseng.Journal of Chromatography A,2012,1231(1231):31-45
[6]Kang C,Lai C J,Zhao D,et al.A practical protocol for comprehensive evaluation of sulfur-fumigation of Gastrodia Rhizoma using metabolome and health risk assessment analysis.Journal of Hazardous Materials,2017,340:221
[7]Sun X,Cui X B,Wen H M,et al.Influence of sulfur fumigation on the chemical profiles of Atractylodes macrocephala Koidz evaluated by UFLC-QTOF-MS combined with multivariate statistical analysis.Journal of Pharmaceutical&Biomedical Analysis,2017,141:19
[8]Kong M,Liu H H,Wu J,et al.Effects of sulfur-fumigation on the pharmacokinetics, metabolites and analgesic activity of Radix Paeoniae Alba.Journal of Ethnopharmacology,2017,212:95-105
[9]Ma X Q,Leung A K,Chan C L,et al.UHPLC UHD Q-TOF MS/MS analysis of the impact of sulfur fumigation on the chemical profile of Codonopsis Radix(Dangshen).Analyst,2014,139(2):505
[10]Cao G,Li Q,Zhang J,et al.A purge and trap technique to capture volatile compounds combined with comprehensive twodimensional gas chromatography/time-of-flight mass spectrometry to investigate the effect of sulfur-fumigation on Radix Angelicae Dahuricae.Biomedical Chromatography Bmc,2014,28(9):1167-1172
[11]Xu S J,Yang L, Zeng X,et al.Characterization of compounds in the Chinese herbal drug Mu-Dan-Pi by liquid chromatography coupled to electrospray ionization mass spectrometry.Rapid Communications in Mass Spectrometry Rcm,2006,20(22):3275-3288
[12]康传志,吕朝耕,蒋靖怡,等.霉变与煎煮对硫熏天麻质量及二氧化硫残留量的影响.中华中医药杂志,2018,33(5):2047-2050
[13]Yan Z,Chen C,Xie X,et al.Rapid screening and quantification of sulfonate derivatives in white peony root by UHPLC-MS-MS.Analytical&Bioanalytical Chemistry,2012,402(6):2173-2182
[14]王巧,郭洪祝,霍长虹,等.白芍加工产物芍药苷亚硫酸酯的提取分离和结构鉴定.“以岭医药杯”全国青年药学工作者最新科研成果交流会论文集,2006