Citation: Wei Pan, Dong-Xiao Yin, Hai-Rong Jing, Hao-Jing Chang, Hao Wen, De-Hai Liang. Core-Corona Structure Formed by Hyaluronic Acid and Poly(L-lysine) via Kinetic Path[J]. Chinese Journal of Polymer Science, ;2019, 37(1): 36-42. doi: 10.1007/s10118-018-2166-z shu

Core-Corona Structure Formed by Hyaluronic Acid and Poly(L-lysine) via Kinetic Path

Beijing National Laboratory for Molecular Sciences and Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China

Corresponding author: De-Hai Liang, dliang@pku.edu.cn
Received Date: 2 May 2018
Revised Date: 26 May 2018
Accepted Date: 28 May 2018
Available Online: 28 June 2018

The structure and kinetics of the complex formed by hyaluronic acid (HA) and poly(L-lysine) (PLL) were studied by time-resolved laser light scattering, TEM, and AFM. Because HA has a hydrophilic backbone, the complexes formed by HA and PLL are different from those formed by oppositely charged polyelectrolytes both having hydrophobic backbones. Instead of forming strong aggregates and even precipitates, the complex in the presence of excess HA is stable in the studied time period. More importantly, the complex spontaneously forms core-corona structure by the rearrangement of HA chains. The core is composed of complex rich of PLL and the corona is mainly HA. Further analysis shows that the hydrogen bond formed by HA creates a barrier hindering the further relaxation of HA chains. The automatic formation of core-corona structure by PLL/HA is helpful not only to understand the relaxation of polyelectrolyte in complex, but also to develop drug carriers with desirable properties.
- Polyelectrolyte complex,
- Core-corona structure,
- Hyaluronic acid,
- Poly(L-lysine),
- Laser light scattering
1. [1]
  Izumrudov, V. A.; Galaev, I. Y.; Mattiasson, B. Polyelectrolyte- potential for bioseparation. Bioseparation 1998, 7(4-5), 207-220. doi: 10.1023/A:1008007818765
2. [2]
  Bolto, B.; Gregory, J. Organic polyelectrolytes in water treatment. Water Res. 2007, 41(11), 2301-2324. doi: 10.1016/j.watres.2007.03.012
3. [3]
  Savage, N.; Diallo, M. S. Nanomaterials and water purification: opportunities and challenges. J. Nanopart. Res. 2005, 7(4-5) 331-342. doi: 10.1007/s11051-005-7523-5
4. [4]
  Zhao, Q.; Zhang, P.; Antonietti, M.; Yuan, J. Poly(ionic liquid) complex with spontaneous micro-/mesoporosity: template-free synthesis and application as catalyst support. J. Am. Chem. Soc. 2012, 134(29), 11852-11855. doi: 10.1021/ja303552p
5. [5]
  Zheng, C.; Niu, L.; Yan, J. J.; Liu, J.; Luo, Y.; Liang, D. H. Structure and stability of the complex formed by oligonucleotides. Phys. Chem. Chem. Phys. 2012, 14(20), 7352-7359. doi: 10.1039/c2cp24086f
6. [6]
  Zhou, J. H.; Liu, J.; Shi, T.; Xia, Y. Q.; Luo, Y.; Liang, D. H. Phase separation of siRNA-polycation complex and its effect on transfection efficiency. Soft Matter 2013, 9(7), 2262-2268. doi: 10.1039/c2sm27498a
7. [7]
  Nomoto, T.; Fukushima, S.; Kumagai, M.; Machitani, K.; Arnida; Matsumoto, Y.; Oba, M.; Miyata, K.; Osada, K.; Nishiyama, N.; Kataoka, K. Three-layered polyplex micelle as a multifunctional nanocarrier platform for light-induced systemic gene transfer. Nat. Commun. 2014, 5, 3545. doi: 10.1038/ncomms4545
8. [8]
  Zheng, C.; Niu, L.; Pan, W.; Zhou, J. H.; Lv, H.; Cheng, J. J.; Liang, D. H. Long-term kinetics of DNA interacting with polycations. Polymer 2014, 55(10), 2464-2471. doi: 10.1016/j.polymer.2014.03.038
9. [9]
  Lee, Y.; Kataoka, K. Biosignal-sensitive polyion complex micelles for the delivery of biopharmaceuticals. Soft Matter 2009, 5(20), 3810-3817. doi: 10.1039/b909934d
10. [10]
  Oh, K. T.; Bronich, T. K.; Bromberg, L.; Hatton, T. A.; Kabanov, A. V. Block ionomer complexes as prospective nanocontainers for drug delivery. J. Control Release 2006, 115(1), 9-17. doi: 10.1016/j.jconrel.2006.06.030
11. [11]
  Mo, R.; Jiang, T.; DiSanto, R.; Tai, W.; Gu, Z. ATP-triggered anticancer drug delivery. Nat. Commun. 2014, 5, 3364. doi: 10.1038/ncomms4364
12. [12]
  Yue, Y.; Wu, C. Progress and perspectives in developing polymeric vectors for in vitro gene delivery. Biomater. Sci. 2013, 1(2), 152-170. doi: 10.1039/C2BM00030J
13. [13]
  Aliabadi, H. M.; Landry, B.; Sun, C.; Tang, T.; Uludag, H. Supramolecular assemblies in functional siRNA delivery: where do we stand? Biomaterials 2012, 33(8), 2546-2569. doi: 10.1016/j.biomaterials.2011.11.079
14. [14]
  Zhou, J. H.; Wen, H.; Su, C. C.; Niu, L.; Liang, D. H. Complexation between DNA and peptides with precisely controlled charge density and distribution. Chinese J. Polym. Sci. 2014, 32(11), 1460-1468. doi: 10.1007/s10118-014-1478-x
15. [15]
  Niu, L.; Yan, J. J.; Yang, X. Y.; Burger, C.; Rong, L. X.; Hsiao, B.; Liang, D. H. Complexation of DNA with cationic surfactants as studied by small-angle X-ray scattering. Sci. China Chem. 2014, 57(12), 1738-1745. doi: 10.1007/s11426-014-5159-y
16. [16]
  Wen, H.; Yin, Y. D.; Huang, C.; Pan, W.; Liang, D. H. Encapsulation of RNA by negatively charged human serum albumin via physical interactions. Sci. China Chem. 2017, 60(1), 130-135. doi: 10.1007/s11426-016-0094-8
17. [17]
  Gummel, J.; Cousin, F.; Boue, F. Counterions release from electrostatic complexes of polyelectrolytes and proteins of opposite charge: a direct measurement. J. Am. Chem. Soc. 2007, 129(18), 5806-5807. doi: 10.1021/ja070414t
18. [18]
  Ha, B. Y.; Liu, A. J. Counterion-mediated attraction between two like-charged rods. Phys. Rev. Lett. 1997, 79(7), 1289-1292. doi: 10.1103/PhysRevLett.79.1289
19. [19]
  Ren, Y.; Jiang, X.; Pan, D.; Mao, H. Q. Charge density and molecular weight of polyphosphoramidate gene carrier are key parameters influencing its DNA compaction ability and transfection efficiency. Biomacromolecules 2010, 11(12), 3432-3439. doi: 10.1021/bm1009574
20. [20]
  Zelikin, A. N.; Izumrudov, V. Polyelectrolyte complexes formed by calf thymus DNA and aliphatic ionenes: Unexpected change in stability upon variation of chain length of ionenes of different charge density. Macromol. Biosci. 2002, 2(2), 78-81. doi: 10.1002/(ISSN)1616-5195
21. [21]
  Stoerkle, D.; Duschner, S.; Heimann, N.; Maskos, M.; Schmidt, M. Complex formation of DNA with oppositely charged polyelectrolytes of different chain topology: cylindrical brushes and, dendrimers. Macromolecules 2007, 40(22), 7998-8006. doi: 10.1021/ma0711689
22. [22]
  Izumrudov, V. A.; Wahlund, P. O.; Gustavsson, P. E.; Larsson, P. O.; Galaev, I. Y. Factors controlling phase separation in water-salt solutions of DNA and polycations. Langmuir 2003, 19(11), 4733-4739. doi: 10.1021/la0206256
23. [23]
  Michaels, A. S.; Miekka, R. G. Polycation-polyanion complexes – preparation and properties of poly-(vinylbenzyltrimethylammonium) poly-(styrenesulfonate). J. Phys. Chem. 1961, 65(10), 1765-1773. doi: 10.1021/j100827a020
24. [24]
  Michaels, A. S. Polyelectrolyte complexes. Ind. Eng. Chem. 1965, 57(10), 32-40. doi: 10.1021/ie50670a007
25. [25]
  Chen, J. H.; Heitmann, J. A.; Hubbe, M. A. Dependency of polyelectrolyte complex stoichiometry on the order of addition. 1. Effect of salt concentration during streaming current titrations with strong poly-acid and poly-base. Colloids Surf. A 2003, 223(1-3), 215-230. doi: 10.1016/S0927-7757(03)00222-X
26. [26]
  Chen, J. H.; Hubbe, M. A.; Heitmann, J. A.; Argyropoulos, D. S.; Rojas, O. J. Dependency of polyelectrolyte complex stoichiometry on the order of addition - 2. Aluminum chloride and poly-vinylsulfate. Colloids Surf. A 2004, 246(1-3), 71-79. doi: 10.1016/j.colsurfa.2004.07.021
27. [27]
  Zhang, R.; Shklovskii, B. T. Phase diagram of solution of oppositely charged polyelectrolytes. Physica A 2005, 352(1), 216-238. doi: 10.1016/j.physa.2004.12.037
28. [28]
  Dias, R. S.; Linse, P.; Pais, A. A. C. C. Stepwise disproportionation in polyelectrolyte complexes. J. Comput. Chem. 2011, 32(12), 2697-2707. doi: 10.1002/jcc.v32.12
29. [29]
  Kizilay, E.; Kayitmazer, A. B.; Dubin, P. L. Complexation and coacervation of polyelectrolytes with oppositely charged colloids. Adv. Colloid Interface Sci. 2011, 167(1-2), 24-37. doi: 10.1016/j.cis.2011.06.006
30. [30]
  Su, C. C.; Zhao, M. T.; Zhu, Z. C.; Zhou, J. H.; Wen, H.; Yin, Y. D.; Deng, Y.; Qiu, D.; Li, B. H.; Liang, D. H. Effect of peptide charge distribution on the structure and kinetics of DNA complex. Macromolecules 2015, 48(3), 756-763. doi: 10.1021/ma501901b
31. [31]
  Fujii, T.; Sun, Y. L.; An, K. N.; Luo, Z. P. Mechanical properties of single hyaluronan molecules. J. Biomech. 2002, 35(4), 527-531. doi: 10.1016/S0021-9290(01)00205-6
32. [32]
  Aruffo, A.; Stamenkovic, I.; Melnick, M.; Underhill, C. B.; Seed, B. CD44 is the principal cell-surface receptor for hyaluronate. Cell 1990, 61(7), 1303-1313. doi: 10.1016/0092-8674(90)90694-A
33. [33]
  Brandrup, J.; Immergut, E. H.; Grulke, E. A. in Polymer handbook. Wiley-Blackwell, New Jersey, 1999.
34. [34]
  Zezin, A. B.; Kabanov, V. A. A new class of complex water-soluble polyelectrolytes. Russ. Chem. Rev. 1982, 51(9), 833-855. doi: 10.1070/RC1982v051n09ABEH002921
35. [35]
  Schärtl, W. in Light scattering from polymer solutions and nanoparticle dispersions. Springer-Verlag, Berlin, 2007.
36. [36]
  Wu, C.; Zhou, S. Q. Laser-light scattering study of the phase-transition of poly(n-isopropylacrylamide) in water. 1. Single-chain. Macromolecules 1995, 28(24), 8381-8387. doi: 10.1021/ma00128a056
37. [37]
  Wang, X. H.; Qiu, X. P.; Wu, C. Comparison of the coil-to-globule and the globule-to-coil transitions of a single poly(N-isopropylacrylamide) homopolymer chain in water. Macromolecules 1998, 31(9), 2972-2976. doi: 10.1021/ma971873p
38. [38]
  Wen, H.; Pan, W.; Zhou, J. H.; Li, Z. C.; Liang, D. H. Complete dissociation and reassembly behavior as studied by using poly(ethylene glycol)-block-poly(glutamate sodium) and kanamycin A. Soft Matter 2015, 11(10), 1930-1936. doi: 10.1039/C4SM02656J
39. [39]
  Voets, I. K.; de Keizer, A.; Stuart, M. A. C. Complex coacervate core micelles. Adv. Colloid Interface Sci. 2009, 147-148, 300-318. doi: 10.1016/j.cis.2008.09.012
40. [40]
  Pergushov, D. V.; Mueller, A. H. E.; Schacher, F. H. Micellar interpolyelectrolyte complexes. Chem. Soc. Rev. 2012, 41(21), 6888-6901. doi: 10.1039/c2cs35135h
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