Self-Assembly of Graphene Oxide at Poly（3-hydroxybutyrate） Microparticles Toward High-performance Intercalated Nanocomposites

doi:10.7503/cjcu20210566

Abstract

Abstract:

As one of the most important natural biopolymers， poly（3-hydroxybutyrate）（PHB） has been identified by an ecofriendly lifecycle from bacterial synthesis to practical processing and recycling， holding great promise in applications for biomedical and packaging materials. However， due to the intrinsic characters including poor self- nucleation capability and excessively large spherulites， the application of PHB is dwarfed by low impact resistance， poor ductility and high creep compliance. Herein， a combination of aqueous processing and confined structuring was proposed to prepare graphene oxide（GO）-intercalated PHB nanocomposites. In specific， GO nanosheets were exfo- liated and dispersed in water， which would encapsulate the submicron PHB microspheres to form the PHB@GO self-assemblies， followed by confined structuring under a high pressure above the melting temperature of PHB. Albeit at an ultralow loading of 0.1%（mass fraction）， the intercalated GO nanosheets showed high capability to enhanced the isothermal and non-isothermal crystallization kinetics of PHB， resulting in highly dense spherulites with a relatively uniform size. An unexcepted brittle-ductile transition was developed in the intercalated nanocomposites， leading to remarkable increase in tensile strength and elongation at break. This was accompanied by significant rise of thermomechanical properties and creep resistance， especially at high temperatures. The flexibility in the choice of functional nanofillers permits broad applications in the fabrication of high-performance PHB-based composites.

Key words: Poly（3-hydroxybutyrate）, Graphene oxide, Intercalated structure, Crystalline morphology, Mechanical property

CLC Number:

O631

TrendMD:

ZHANG Zhibo, SHANG Han, XU Wenxuan, HAN Guangdong, CUI Jinsheng, YANG Haoran, LI Ruixin, ZHANG Shenghui, XU Huan. Self-Assembly of Graphene Oxide at Poly（3-hydroxybutyrate） Microparticles Toward High-performance Intercalated Nanocomposites[J]. Chem. J. Chinese Universities, 2022, 43(2): 20210566.

Figures/Tables 9

Fig.1 Digital photos of the aqueous solutions before(A) and after(B) mechanical stirring and SEM images of pristine PHB microparticles(C) and PHB@GO hybrids(D—F)

Fig.2 Digital photos of GO0(A) and GO0.1(B) and TEM image of the dispersion morphology of GO in the composite film(C)

Fig.3 Plots of relative crystallinity versus the crystallization time for GO0(a) and GO0.1(b) during isothermal crystallization at 100(A), 110(B) and 120 ℃(C)The values of half-time crystallization(t1/2) are marked.

Fig.4 POM images of GO0(A1—A3, B1—B3) and GO0.1(C1—C3, D1—D3) after isothermal crystallization at 100(A1—D1), 110(A2—D2) and 120 ℃(A3—D3) for 30 min

Fig.5 POM images of GO0(A1—A3, B1—B3) and GO0.1(C1—C3, D1—D3) after non?isothermal melt crystallization with a cooling rate of 5(A1—D1), 10(A2—D2) and 20 ℃/min(A3—D3)

Fig.6 Typical stress?strain curves of GO0 and GO0.1(A—C) with different crosshead speed and SEM images of fracture surfaces after tensile failure of GO0(D—F) and GO0.1(G—I) with different crosshead speed

Fig.7 DMA?measured creep compliance?time curves(A—C) and creep and creep-recovery curves(D—F) of GO/PHB composites at 25 ℃(A, D), 60 ℃(B, E) and 100 ℃(C, F)

Fig.8 Dynamic storage modulus of GO0 and GO0.1

Fig.9 Derivative thermogra vimetry(DTG) curves(A) and TGA curves(B) for GO/PHB composites

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