天然聚多糖的溶解机理及溶液性质

汪森; 张蓉蓉; 许小娟; 吕昂; 张俐娜

doi:10.11777/j.issn1000-3304.2017.17108

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天然聚多糖的溶解机理及溶液性质

专论 | 更新时间：2021-01-27

- 天然聚多糖的溶解机理及溶液性质
- Dissolution Mechanism and Solution Properties of Natural Polysaccharides
- 高分子学报 2017年第9期页码：1426-1443
- 作者机构：
  
  武汉大学化学与分子科学学院武汉 430072
- 作者简介：
  
  [ "吕昂，男，1983年4月生.武汉大学化学与分子科学学院副教授. 2009年毕业于武汉大学化学与分子科学学院并获得理学博士学位，2010年至2013年分别在美国加州大学戴维斯分校和加拿大阿尔伯塔大学从事联合培养博士后工作，研究生物质大分子的纳米化技术以及纤维素纳米晶须的溶液、流变性质及其与高分子链的相互作用. 2013年6月进入武汉大学化学与分子科学学院从事天然高分子方面的研究工作.主要研究方向难溶性天然高分子在水体系中的溶解及相互作用、高分子溶液行为、氢键体系的拆分与重建" ]
  [ "张俐娜，女，1940年8月生.武汉大学化学与分子科学学院教授/博导，中国科学院院士. 1963年毕业于武汉大学化学系，1985年曾获日本政府学术振兴协会奖学金(JSPS)赴大阪大学研究近2年. 1993年创立天然高分子科研组. 2011年当选中国科学院院士，2014年为英国皇家化学会会士.现任美国化学会刊物 < ACS Sustainable Chemistry & Engineering > 的副主编以及多家国内外刊物编委.基础研究成果已在国内外刊物发表论文600余篇，其中560余篇发表在国际SCI源刊上，被他人引用15000次以上；主编专著15部；获准专利100余项；荣获国家自然科学奖二等奖1项，省级自然科学一等奖1项及技术发明一等奖1项；获美国化学会2011年Anselme Payen奖(国际纤维素与可再生资源材料领域最高奖).曾获全国优秀教师和全国先进工作者等国家级荣誉.主要研究方向高分子物理、天然高分子改性材料、复杂多糖的分子和链构象与其生物活性关系" ]
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2017.17108
  中图分类号：
- 纸质出版日期：2017-9，
  
  收稿日期：2017-4-26，
  
  修回日期：2017-6-1，
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汪森, 张蓉蓉, 许小娟, 吕昂, 张俐娜. 天然聚多糖的溶解机理及溶液性质[J]. 高分子学报, 2017,(9):1426-1443.

Sen Wang, Rong-rong Zhang, Xiao-juan Xu, Ang Lu, Li-na Zhang. Dissolution Mechanism and Solution Properties of Natural Polysaccharides[J]. Acta Polymerica Sinica, 2017,(9):1426-1443.
汪森, 张蓉蓉, 许小娟, 吕昂, 张俐娜. 天然聚多糖的溶解机理及溶液性质[J]. 高分子学报, 2017,(9):1426-1443. DOI： 10.11777/j.issn1000-3304.2017.17108.

Sen Wang, Rong-rong Zhang, Xiao-juan Xu, Ang Lu, Li-na Zhang. Dissolution Mechanism and Solution Properties of Natural Polysaccharides[J]. Acta Polymerica Sinica, 2017,(9):1426-1443. DOI： 10.11777/j.issn1000-3304.2017.17108.

摘要

21世纪"绿色"化学已成为各国科学界和工业界研究与开发的方向.天然高分子中纤维素、甲壳素等聚多糖来源丰富，是重要的可再生资源，也是未来主要的化工原料之一.由于大量的分子内和分子间氢键，它们的溶解长期以来都是非常棘手的问题.另一方面，聚多糖的结构非常复杂，只有弄清楚其链构象和溶液性质，才可能进行合理的分子设计，实现其更好的应用.本文简要介绍了本课题组用碱/尿素水体系低温溶解纤维素和甲壳素等天然高分子的机理和溶液中分子链构象，以及活性多糖在水溶液中的链构象和溶液性质的研究进展.

Abstract

Naturalpolymers such as cellulose

chitin

chitosan and other fungi polysaccharides are derived from renewable resources

which is one kind of main chemical raw materials in the future. The numerous intermolecular and intramolecular hydrogen bonds have made their dissolution difficult in most common solvents. Moreover

their structures are very complex. Clarifying their chain conformation and solution properties is essential in designing their molecular structure

realizing more sophisticated applications. This article introduces the recent results about low temperature dissolution of cellulose

chitin and chitosanin in alkali/urea aqueous solution and their chain conformation and solution properties

as well as solution properties of the active polysaccharides. Cellulose can be dissolved in 7 wt% NaOH-12 wt% urea aqueous solution with precooling (-12℃) within 2 min

whereas chitin can be dissolved in a mixture of NaOH

urea and water atweight ratio of 11:4:85 at -30℃. The weight average molecular weight (

)

radii of gyration (〈

〉

)

hydrodynamic radii (〈

〉

)

the structure-sensitive parameter (

) and persistent length (

) values of the natural macromolecules were determined

indicating the worm-like stiff chain conformation of cellulose

chitin and chitosan. Furthermore

TEM

cryo-TEM and AFM images provide direct observation of the extended chain conformation and the visualized nanofibers constructed from the stiff chains in parallel aggregation in the aqueous solution. A water-soluble neutral polysaccharide (AF1) was extracted from

auricula

judae

was and identified as a high branched

-(1→3)-D-glucan. AF1 was proved to exist as stiff chains in water

and as flexible chains in dimethylsulfoxide (DMSO). The high-branched glucan was used to self-assemble into hollow nanofibers with apparent average diameter of 92 nm. Lentinan

-(1→3)-D-glucan isolated from

Lentinus edodes

exhibited good water solubility

and existed as a triple-helical conformation in the aqueous solution at 25℃. AFM images confirmed that the triple-helical chain conformation of lentinan with high

formed wormlike patterns in aqueous solution at 25℃. Water-insoluble polysaccharide (TM3a)

extracted from sclerotia of

Pleurotus tuber

regium

was identified as ahyperbranched

-D-glucan. The degree of branching of TM3a was 65.5%. The dependence of intrinsic viscosity ([

])

radius of gyration (〈

〉

1/2

)

and hydradynamic radius (

) on the weight-average molecular weight (

) was studied

indicating that TM3a existed as a compact chain conformation with a sphere-like structure in LiCl/DMSO solution. Furthermore

TEM image provided direct observation of the sphere-like pattern of the chain conformation.

关键词

天然高分子低温溶解溶液性质

Keywords

Natural polysaccharidesDissolution at low temperatureSolution propertiesChain conformationMolecular weight

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