蒲公英提取物-茶多酚-玉米秸秆纤维素抗菌复合膜制备与性能

张群利; 邬泽凯; 崔琳琳; 谢文静; 于启蒙; 刘宇鹏

doi:10.13801/j.cnki.fhclxb.20221215.001

蒲公英提取物-茶多酚-玉米秸秆纤维素抗菌复合膜制备与性能

doi: 10.13801/j.cnki.fhclxb.20221215.001

1.
东北林业大学　工程技术学院，哈尔滨 150040
2.
哈尔滨商业大学　药学院，哈尔滨 150076
3.
森林持续经营与环境微生物工程黑龙江省重点实验室，哈尔滨 150040

基金项目: 中央高校基本科研业务费专项资金(2572019 BL01)

详细信息

通讯作者:
张群利，博士，副教授，硕士生导师，研究方向为功能性包装材料　E-mail: zhangqunli@nefu.edu.cn

中图分类号: TS71+1；TB332
计量
- 文章访问数: 562
- HTML全文浏览量: 293
- PDF下载量: 18
- 被引次数: 0
出版历程
- 收稿日期: 2022-10-19
- 修回日期: 2022-11-22
- 录用日期: 2022-12-09
- 网络出版日期: 2022-12-19
- 刊出日期: 2023-09-15

Preparation and performance of cellulose antibacterial composite film from corn stover with dandelion extract and tea polyphenols

1.
College of Engineering and Technology, Northeast Forestry University, Harbin 150040, China
2.
School of Pharmacy, Harbin University of Commerce, Harbin 150076, China
3.
Key Laboratory of Sustainable Forest Management & Environmental Microbiology in Heilongjiang Province, Harbin 150040, China

Funds: Fundamental Research Funds for the Central Universities (2572019 BL01)

摘要

摘要: 玉米秸秆的高附加值利用既可以减轻污染和资源浪费，还对探索秸秆的工业化利用和农业可持续发展具有深远的意义。以玉米秸秆制备的微晶纤维素(CSMCC)为原料，1-丁基-3-甲基咪唑氯盐([Bmim]Cl)为溶剂体系，蒲公英提取物(DE)和茶多酚(TP)为抗菌剂，通过共混法制备抗菌复合膜。通过FTIR、XRD、SEM和热重分析对复合膜的形貌和结构进行表征及对力学、光学、阻隔、抑菌等性能测试分析。结果表明：DE和TP与纤维素基膜较好地复合，复配抗菌剂DE-TP抗菌复合膜相比于DE、TP抗菌复合膜具有较优的拉伸强度((52.60±6.33) MPa)、氧气阻隔性能(氧气透过系数为(1.65±0.25)×10⁻¹¹ cm³·cm/(cm²·s·Pa))，且对大肠杆菌和金黄色葡萄球菌具有更好的抑制作用。同时DE-TP抗菌复合膜断裂伸长率相比于纤维素基膜提升了53.96%，透光率保持在(82.56±0.26)%，具有良好的力学性能和光学性能。为制备对控制食品腐败变质和生物资源高效利用具有重要意义的环境友好型抗菌复合膜的研发提供新思路。
- 纤维素 /
- 蒲公英 /
- 茶多酚 /
- 力学性能 /
- 光学性能 /
- 阻隔性能 /
- 抑菌性能 /
- 功能材料
Abstract: The high value-added utilization of corn straw can not only reduce pollution and resource waste, but also has far-reaching significance for exploring the industrial utilization of corn straw and sustainable agricultural development. Using microcrystalline cellulose (CSMCC) prepared from corn straw as raw material, 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) as solvent system, dandelion extract (DE) and tea polyphenol (TP) as antibacterial agents, antibacterial composite film was prepared by blending method. The morphology and structure of the composite film were characterized by FTIR, XRD, SEM and thermogravimetric analysis, and the mechanical, optical, barrier and antibacterial properties were tested and analyzed. The results show that DE and TP are well combined with cellulose base film. The composite antibacterial agent DE-TP antibacterial composite film has better tensile strength ((52.60±6.33) MPa), oxygen barrier performance (oxygen transmission coefficient is (1.65±0.25)×10⁻¹¹ cm³·cm/(cm²·s·Pa)) and better inhibition effect on Escherichia coli and Staphylococcus aureus than the DE and TP antibacterial composite films. At the same time, compared with the cellulose base film, elongation at break of DE-TP antibacterial composite film increased by 53.96%, and the light transmittance is (82.56±0.26)%, which has good mechanical and optical properties. It provides a new idea for the research and development of environment-friendly antibacterial composite film, which is important for controlling food spoilage and efficient utilization of biological resources.
- cellulose /
- dandelion /
- tea polyphenol /
- mechanical properties /
- optical properties /
- barrier properties /
- bacteriostatic properties /
- functional materials

HTML全文

图 1 玉米秸秆微晶纤维素(CSMCC) 0^# (a) 和1^# (b)、2^# (c)、3^# (d) 抗菌复合膜图

Figure 1. Pictures of microcrystalline cellulose prepared from corn straw (CSMCC) 0^# (a) and 1^# (b), 2^# (c), 3^# (d) antibacterial composite film

下载: 全尺寸图片幻灯片

图 2 抗菌复合膜制备工艺及评价

Figure 2. Preparation and evaluation of antibacterial composite film

CSC—Corn straw cellulose; DE—Dandelion extract; TP—Tea polyphenols; CSRGC—Corn stalk regenerated cellulose

下载: 全尺寸图片幻灯片

图 3 CSMCC和市购微晶纤维素(MCC)的FTIR图谱

Figure 3. FTIR spectra of CSMCC and commercial microcrystalline cellulose (MCC)

下载: 全尺寸图片幻灯片

图 4 CSMCC和MCC的XRD图谱

Figure 4. XRD patterns of CSMCC and MCC

下载: 全尺寸图片幻灯片

图 5 DE、TP、CSRGC和抗菌复合膜FTIR图谱

Figure 5. FTIR spectra of DE, TP, CSRGC and antibacterial composite film

下载: 全尺寸图片幻灯片

图 6 CSRGC和抗菌复合膜的XRD图谱

Figure 6. XRD patterns of CSRGC and antibacterial composite film

下载: 全尺寸图片幻灯片

图 7 CSRGC 0^#(a) 和1^#(b)、2^#(c)、3^#(d) 抗菌复合膜表面的SEM图像

Figure 7. SEM images of surface of CSRGC 0^#(a) and 1^#(b), 2^#(c), 3^#(d) antibacterial composite film

下载: 全尺寸图片幻灯片

图 8 CSRGC 0^#(a) 和1^# (b)、2^#(c)、3^# (d) 抗菌复合膜的断面SEM图像

Figure 8. SEM images of section of CSRGC 0^#(a) and 1^#(b), 2^#(c), 3^#(d) antibacterial composite film

下载: 全尺寸图片幻灯片

图 9 CSRGC和抗菌复合膜TG曲线

Figure 9. TG curves of CSRGC and antibacterial composite film

下载: 全尺寸图片幻灯片

图 10 CSRGC和抗菌复合膜DTG曲线

Figure 10. DTG diagram of CSRGC and antibacterial composite film

下载: 全尺寸图片幻灯片

图 11 CSRGC和抗菌复合膜的透光率和雾度

Figure 11. Light transmittance and haze of CSRGC and antibacterial composite film

下载: 全尺寸图片幻灯片

表 1 抗菌复合膜组分

Table 1. Composition of antibacterial composite film

Sample	DE content/ wt%	TP content/ wt%	Remarks
0^#	—	—	As blank group
1^#	15	15	w(DE)∶w(TP)=1∶1
2^#	30	—
3^#	—	30
Notes: DE—Dandelion extract; TP—Tea polyphenol; "—" means not added; The added amount of DE and TP is the percentage of the mass of DE and TP in the mass of CSMCC.

下载: 导出CSV

表 2 CSRGC和抗菌复合膜的失重情况

Table 2. Mass loss of CSRGC and antibacterial composite film

Sample	T_5%/℃	T_10%/℃	T_30%/℃	T_50%/℃
0^#	271.1	276.1	288.1	299.1
1^#	235.5	277.5	310.3	326.0
2^#	217.0	261.9	283.6	295.6
3^#	66.5	244.8	275.2	289.9
Note: T_5%, T_10%, T_30%, T_50%—Corresponding temperature when mass loss rate is 5wt%, 10wt%, 30wt%, 50wt%.

下载: 导出CSV

表 3 抗菌复合膜的力学性能

Table 3. Mechanical properties of antibacterial composite film

Sample	TS/MPa	EAB/%	EM/GPa
0^#	99.35±10.56^a	8.97±0.90^c	11.08±0.64^a
1^#	52.60±6.33^b	13.81±1.76^ab	3.82±0.32^b
2^#	50.83±5.04^b	11.57±1.88^bc	4.49±0.94^b
3^#	42.21±4.82^b	15.51±2.43^a	2.78±0.50^c
Notes: TS—Tensile strength; EAB—Elongation at break; EM—Elastic modulus; Different letters represent significant differences (P＜0.05); a, b, c, d—Significant differences between groups.

下载: 导出CSV

表 4 CSRGC和抗菌复合膜的阻隔性能

Table 4. Barrier properties of CSRGC and antibacterial composite film

Sample	OTC/[cm³·cm·(cm²·s·Pa)^-1]
0^#	(3.13±0.99)×10^{−12 d}
1^#	(1.65±0.25)×10^{−11 b}
2^#	(2.11±0.29)×10^{−11 a}
3^#	(2.22±0.11)×10^{−11 a}
Notes: OTC—Oxygen transmission coefficient; Different letters represent significant differences (P＜0.05).

下载: 导出CSV

表 5 抗菌复合膜抑菌性能

Table 5. Antibacterial properties of composite film

Sample	E. coli/mm	S. aureus/mm
0^#	0^d	0^d
1^#	15.22±0.15^a	15.86±0.25^a
2^#	11.32±0.12^c	14.29±0.25^b
3^#	14.11±0.15^b	11.16±0.11^c
Notes: E. coli—Escherichia coli; S. aureus—Staphylococcus aureus; Different letters represent significant differences (P＜0.05).

下载: 导出CSV

参考文献(33)

[1]	ALMEIDA A P C, CANEJO J P, FERNANDES S N, et al. Cellulose-based biomimetics and their applications[J]. Advanced Materials,2018,30(19):1703655. doi: 10.1002/adma.201703655
[2]	AHMED J, GULTEKINOGLU M, EDIRISINGHE M. Bacterial cellulose micro-nano fibres for wound healing applications[J]. Biotechnology Advances,2020,41:107549. doi: 10.1016/j.biotechadv.2020.107549
[3]	曹延娟, 辛斌杰, 张杰, 等. 天然纤维素/聚丙烯腈抗菌纳米纤维的制备与表征[J]. 复合材料学报, 2015, 32(4):1042-1052. doi: 10.13801/j.cnki.fhclxb.20141204.003 CAO Yanjuan, XIN Binjie, ZHANG Jie, et al. Preparation and characterization of natural cellulose/polyacrylonitrile antibacterial nanofibers[J]. Acta Materiae Compositae Sinica,2015,32(4):1042-1052(in Chinese). doi: 10.13801/j.cnki.fhclxb.20141204.003
[4]	王小燕, 刘利, 曾秀, 等. 载Ag改性桑枝韧皮纤维素/聚乙烯醇复合膜的制备及表征[J]. 复合材料学报, 2019, 36(11):2502-2508. doi: 10.13801/j.cnki.fhclxb.20190412.003 WANG Xiaoyan, LIU Li, ZENG Xiu, et al. Preparation and characterization of Ag-carried tetracycline-mulberry bast carboxymethyl cellulose/polyvinyl alcohol composite films[J]. Acta Materiae Compositae Sinica,2019,36(11):2502-2508(in Chinese). doi: 10.13801/j.cnki.fhclxb.20190412.003
[5]	王丽莉, 欧阳土龙, 戴兴兴, 等. 过氧化氢漂白富纤维素材料制备透明纤维素膜研究[J]. 森林工程, 2018, 34(1):41-45,59. doi: 10.3969/j.issn.1006-8023.2018.01.010 WANG Lili, OUYANG Tulong, DAI Xingxing, et al. Preparation of transparent cellulose membrane by hydrogen peroxide bleaching of cellulose-rich materials[J]. Forest Engineering,2018,34(1):41-45,59(in Chinese). doi: 10.3969/j.issn.1006-8023.2018.01.010
[6]	SU Y Q, YANG B, LIU J G, et al. Prospects for replacement of some plastics in packaging with lignocellulose materials: A brief review[J]. Bioresources,2018,13(2):4550-4576.
[7]	ZHANG W L, ZHANG Y Q, CAO J K, et al. Improving the performance of edible food packaging films by using nanocellulose as an additive[J]. International Journal of Biological Macromolecules,2021,166:288-296. doi: 10.1016/j.ijbiomac.2020.10.185
[8]	ABDUL KHALIL H P S, TYE Y Y, SAURABH C K, et al. Biodegradable polymer films from seaweed polysaccharides: A review on cellulose as a reinforcement material[J]. Express Polymer Letters,2017,11(4):244-265. doi: 10.3144/expresspolymlett.2017.26
[9]	WU Y H, LUO X G, LI W, et al. Green and biodegradable composite films with novel antimicrobial performance based on cellulose[J]. Food Chemistry,2016,197:250-256. doi: 10.1016/j.foodchem.2015.10.127
[10]	ZHAO G L, LYU X M, LEE J, et al. Biodegradable and transparent cellulose film prepared eco-friendly from durian rind for packaging application[J]. Food Packaging and Shelf Life,2019,21:100345. doi: 10.1016/j.fpsl.2019.100345
[11]	XU J Y, KRIETEMEYER E F, BODDU V M, et al. Production and characterization of cellulose nanofibril (CNF) from agricultural waste corn stover[J]. Carbohydrate Polymers,2018,192:202-207. doi: 10.1016/j.carbpol.2018.03.017
[12]	YANG K, ZHANG Y J. Reversal of heavy metal-induced antibiotic resistance by dandelion root extracts and taraxasterol[J]. Journal of Medical Microbiology,2020,69:1049-1061. doi: 10.1099/jmm.0.001226
[13]	NOWAK A, DUCHNIK W, ZIELONKA-BRZEZICKA J, et al. The antioxidant activity of ethanolic and aqueous extracts of dandelion (Taraxacum officinale L.)[J]. Pomeranian Journal of Life Sciences,2019,65(4):83-88.
[14]	马艳妮, 魏悦, 李智宁, 等. 蒲公英根活性组分体外抗菌及抗炎作用[J]. 食品与发酵工业, 2022, 48(1):98-103. doi: 10.13995/j.cnki.11-1802/ts.027693 MA Yanni, WEI Yue, LI Zhining, et al. In vitro antibacterial and anti-inflammatory activity of active components from dandelion root[J]. Food and Fermentation Industries,2022,48(1):98-103(in Chinese). doi: 10.13995/j.cnki.11-1802/ts.027693
[15]	吴颖, 刘晴, 唐文, 等. 丹参挥发油与蒲公英提取物复配物在化妆品中的应用[J]. 精细化工, 2022, 39(3):562-568. doi: 10.13550/j.jxhg.20210806 WU Ying, LIU Qing, TANG Wen, et al. Application of complexes of Salvia miltiorrhiza volatile oil and dandelion extract in cosmetics[J]. Fine Chemicals,2022,39(3):562-568(in Chinese). doi: 10.13550/j.jxhg.20210806
[16]	何惠利, 任雪娇, 张莉力. 蒲公英黄酮-壳聚糖复合膜的制备及对冷鲜鸡胸肉保鲜的研究[J]. 食品研究与开发, 2022, 43(7):112-118. doi: 10.12161/j.issn.1005-6521.2022.07.016 HE Huili, REN Xuejiao, ZHANG Lili. Preparing dandelion flavonoids-chitosan composite membrane to preserve chilled chicken breast[J]. Food Research and Development,2022,43(7):112-118(in Chinese). doi: 10.12161/j.issn.1005-6521.2022.07.016
[17]	YAN Z M, ZHONG Y Z, DUAN Y H, et al. Antioxidant mechanism of tea polyphenols and its impact on health benefits[J]. Animal Nutrition,2020,6(2):115-123. doi: 10.1016/j.aninu.2020.01.001
[18]	ZHANG W L, JIANG H T, RHIM J W, et al. Tea polyphenols (TP): A promising natural additive for the manufacture of multifunctional active food packaging films[J]. Critical Reviews in Food Science and Nutrition,2023,63(2):288-301.
[19]	LUO J J, ZUO D Q, DENG Z H, et al. Effects of heat treatment and tea polyphenols on the structure and properties of polyvinyl alcohol nanofiber films for food packaging[J]. Coatings,2020,10(1):49. doi: 10.3390/coatings10010049
[20]	LIU Y W, WANG S Y, LAN W J, et al. Development of ultrasound treated polyvinyl alcohol/tea polyphenol composite films and their physicochemical properties[J]. Ultrasonics Sonochemistry,2019,51:386-394. doi: 10.1016/j.ultsonch.2018.07.043
[21]	ZHANG W L, JIANG W B. Antioxidant and antibacterial chitosan film with tea polyphenols-mediated green synthesis silver nanoparticle via a novel one-pot method[J]. International Journal of Biological Macromolecules,2020,155:1252-1261. doi: 10.1016/j.ijbiomac.2019.11.093
[22]	蔡月, 王梦军, 年琳玉, 等. 茶多酚@沸石咪唑酯骨架材料/壳聚糖/海藻酸钠活性包装膜的制备及表征[J]. 食品科学, 2022, 43(17):272-281. doi: 10.7506/spkx1002-6630-20220217-123 CAI Yue, WANG Mengjun, NIAN Linyu, et al. Preparation and characterization of tea polyphenols@zeolitic imidazolate framework-8/chitosan/sodium alginate active packaging film[J]. Food Science,2022,43(17):272-281(in Chinese). doi: 10.7506/spkx1002-6630-20220217-123
[23]	ZHANG D, CHEN L, CAI J, et al. Starch/tea polyphenols nanofibrous films for food packaging application: From facile construction to enhance mechanical, antioxidant and hydrophobic properties[J]. Food Chemistry,2021,360:129922. doi: 10.1016/j.foodchem.2021.129922
[24]	GAO L P, ZHU T, HE F Y, et al. Preparation and characterization of functional films based on chitosan and corn starch incorporated tea polyphenols[J]. Coatings,2021,11(7):817. doi: 10.3390/coatings11070817
[25]	梁杰, 蔡力锋, 刘涛, 等. 茶多酚对海藻酸钠/玉米淀粉复合膜的影响及保鲜应用[J]. 食品研究与开发, 2022, 43(1):7-16. doi: 10.12161/j.issn.1005-6521.2022.01.002 LIANG Jie, CAI Lifeng, LIU Tao, et al. Effect of tea polyphenols on sodium alginate/corn starch composite film and its application in freshness preservation[J]. Food Research and Development,2022,43(1):7-16(in Chinese). doi: 10.12161/j.issn.1005-6521.2022.01.002
[26]	顾晓华, 李燕, 刘思雯, 等. 茶多酚-聚乳酸/聚碳酸丁二醇酯抗菌复合纤维膜的制备及性能[J]. 复合材料学报, 2020, 37(6):1227-1233. doi: 10.13801/j.cnki.fhclxb.20190929.002 GU Xiaohua, LI Yan, LIU Siwen, et al. Preparation and properties of tea polyphenol-polylactic acid/polybutylene carbonate antibacterial composite fiber membrane[J]. Acta Materiae Compositae Sinica,2020,37(6):1227-1233(in Chinese). doi: 10.13801/j.cnki.fhclxb.20190929.002
[27]	王博, 巩涵, 畅鹏, 等. 细菌纤维素-茶多酚复合膜的特性及结构[J]. 食品科学, 2018, 39(17):229-235. doi: 10.7506/spkx1002-6630-201817037 WANG Bo, GONG Han, CHANG Peng, et al. Properties and structure of bacterial cellulose-tea polyphenol composite film[J]. Food Science,2018,39(17):229-235(in Chinese). doi: 10.7506/spkx1002-6630-201817037
[28]	CHEN F, CHI C D. Development of pullulan/carboxylated cellulose nanocrystal/tea polyphenol bionanocomposite films for active food packaging[J]. International Journal of Biological Macromolecules,2021,186:405-413. doi: 10.1016/j.ijbiomac.2021.07.025
[29]	中国国家标准化管理委员会. 塑料拉伸性能的测定第3部分: 薄膜和薄片的实验条件: GB/T 1040.3—2006[S]. 北京: 中国标准出版社, 2006. Standardization Administration of the People’s Republic of China. Plastics—Determination of tensile properties—Part 3: Test conditions for films and sheets: GB/T 1040.3—2006[S]. Beijing: China Standards Press, 2006(in Chinese).
[30]	中国国家标准化管理委员会. 透明塑料透光率和雾度的测定: GB/T 2410—2008[S]. 北京: 中国标准出版社, 2008. Standardization Administration of the People’s Republic of China. Determination of the luminous transmittance and haze of transparent plastics: GB/T 2410—2008[S]. Beijing: China Standards Press, 2008(in Chinese).
[31]	中国国家标准化管理委员会. 塑料薄膜和薄片气体透过性试验方法压差法: GB/T 1038—2000[S]. 北京: 中国标准出版社, 2000. Standardization Administration of the People’s Republic of China. Plastics—Film and sheeting—Determination of gas transmission—Differential-pressure method: GB/T 1038—2000[S]. Beijing: China Standards Press, 2000(in Chinese).
[32]	蓝蔚青, 杜金涛, 梅俊, 等. 茶多酚抑菌机制及在水产品保鲜中的应用进展[J]. 包装工程, 2021, 42(5):73-79. LAN Weiqing, DU Jintao, MEI Jun, et al. Research progress on antibacterial mechanism of tea polyphenol and its application in preservation of aquatic products[J]. Packaging Engineering,2021,42(5):73-79(in Chinese).
[33]	张强, 胡维岗, 金新文. 壳聚糖-蒲公英提取物的抑菌活性与稳定性研究[J]. 食品工业科技, 2015, 36(20):150-154. doi: 10.13386/j.issn1002-0306.2015.20.023 ZHANG Qiang, HU Weigang, JIN Xinwen. Study on antibacterial activity and stability of chitosan and dandelion extract[J]. Science and Technology of Food Industry,2015,36(20):150-154(in Chinese). doi: 10.13386/j.issn1002-0306.2015.20.023