基于芳香基双硫键的乙酸酯化纳米纤维素/聚(脲-氨酯)自愈合材料
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摘要
基于芳香基双硫键,以聚丙二醇-4000(PPG-4000)和异佛尔酮二异氰酸酯(IPDI)为原料,双(4-氨基苯基)硫醚为交联剂,乙酸酯化纳米纤维素作为增强相,制备得到乙酸酯化纳米纤维素/聚(脲-氨酯)[esterified cellulose nanocrystals/poly(urea-urethane),E-CNCs/Pus]自愈合复合材料。对其力学性能、热学性能、表面化学结构、自愈合性能进行了表征研究。结果表明,E-CNCs/PUs在室温下不需其他额外条件即可实现自愈合,说明芳香基双硫键可作为动态交联键应用于自愈合聚(脲-氨酯)的设计与构建;E-CNCs添加量为0.1%时,其聚(脲-氨酯)复合材料拉伸强度达到5.71MPa,与纯聚(脲-氨酯)材料相比,增加了43.11%;E-CNCs/PUs复合材料不仅具有较高的拉伸强度,而且保持了良好的弹性和延展性;热学性能分析结果表明,E-CNCs对聚(脲-氨酯)复合材料热稳定性具有较小影响。
In this study,the esterified cellulose nanocrystals/poly(urea-urethane)(E-CNCs/PUs)self-healing materials were prepared using polypropylene glycol 4000(PPG-4000)and isophorone diisocyanate(IPDI)as raw material,bis(4-aminophenyl) sulfide as crosslinking agent,and esterified cellulose nanocrystals as reinforcement. The mechanical properties,thermal properties,surface chemical structures,and self-healing properties were investigated. The results show that E-CNCs/PUs were self-healing effectively at room temperature without any external interventions,which confirms that bis(4-aminophenyl) disulfide can be effectively used as a dynamic cross-linker for the design of self-healing poly(urea-urethane) material. The maximum tensile strength of E-CNCs/PUs could reach 5.71 MPa when the additive amount of E-CNCs was 0.1%,which was increased by 43.11% compared with pure poly(urea-urethane). E-CNCs/PUs composite materials present high tensile strength,elasticity,and malleability. The additive of E-CNCs just has a small influence on the thermal properties of E-CNCs/PUs self-healing materials.
In this study,the esterified cellulose nanocrystals/poly(urea-urethane)(E-CNCs/PUs)self-healing materials were prepared using polypropylene glycol 4000(PPG-4000)and isophorone diisocyanate(IPDI)as raw material,bis(4-aminophenyl) sulfide as crosslinking agent,and esterified cellulose nanocrystals as reinforcement. The mechanical properties,thermal properties,surface chemical structures,and self-healing properties were investigated. The results show that E-CNCs/PUs were self-healing effectively at room temperature without any external interventions,which confirms that bis(4-aminophenyl) disulfide can be effectively used as a dynamic cross-linker for the design of self-healing poly(urea-urethane) material. The maximum tensile strength of E-CNCs/PUs could reach 5.71 MPa when the additive amount of E-CNCs was 0.1%,which was increased by 43.11% compared with pure poly(urea-urethane). E-CNCs/PUs composite materials present high tensile strength,elasticity,and malleability. The additive of E-CNCs just has a small influence on the thermal properties of E-CNCs/PUs self-healing materials.
引文
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[2]GUIMARD N K,OEHLENSCHLAEGER K K,ZHOU J,et al.Current trends in the field of self-healing materials[J].Macromolecular Chemistry and Physics,2012,213:131-143.
[3]BURATTINI S,GREENLAND B W,MERINO D H,et al.A healable supramolecular polymer blend based on aromaticπ-πstacking and hydrogen-bonding interactions[J].Journal of the American Chemistry Society,2010,132,12051-12058.
[4]DELEBECQ E,PASCAULT J P,BOUTEVIN B,et al.On the versatility of urethane/urea bonds:reversibility,blocked isocyanate,and non-isocyanate polyurethane[J].Chemical Reviews,2013,113,80-118.
[5]刘璇璇.基于热可逆Diels-Alder反应的自修复线型聚氨酯的研究[D].上海:上海交通大学,2013.LIU X X Study of self-healing polyurethane based on thermoreversible Diels-Alder reaction[D].Shanghai:Shanghai Jiao Tong University,2013.
[6]GHOSH B,URBAN M W.Self-repairing oxetane-substituted chitosan polyurethane networks[J].Science,2009,323:1458-1460.
[7]AMAMOTO Y,OTSUKA H,TAKAHARA A,et al.Self-healing of covalently cross-linked polymers by reshuffling thiuram disulfide moieties in air under visible light[J].Advanced Materials,2012,24:3975-3980.
[8]MEYER C D,JOINER C S,STODDART F.Template-directed synthesis employing reversible imine bond formation[J].Chemical Society Reviews,2007,36,1705-1723.
[9]张云飞,邓国华.基于动态共价键的可自愈合聚合物凝胶[J].化工进展,2012,31(10):2239-2244.ZHANG Y F,DENG G H.Self-healing polymer gels based on dynamic covalent bonds[J].Chemical Industry and Engineering Progress,2012,31(10):2239-2244.
[10]YUAN Y C,RONG M Z,ZHANG M Q,et al.Self-healing polymeric materials using epoxy/mercaptan as the healant[J].Macromolecules,2008,41:5197-5202.
[11]OTSUKA H,NAGANO S,KOBASHI Y,et al.A dynamic covalent polymer driven by disulfide metathesis under photoirradiation[J].Chemical Communications,2010,46:1150-1152.
[12]REKONDO A,MARTIN R,DE LUZURIAGA A R,et al.Catalyst-free room-temperature self-healing elastomers based on aromatic disulfide metathesis[J].Materials Horizons,2014,1:237-240.
[13]林凤采,卢麒麟,林咏梅,等.一步法制备乙酰化纳米纤维素及其性能表征[J].化工进展,2016,35(2):559-564.LIN F C,LU Q L,LIN Y M,et al.Preparation and characterization of acetylated nanocellulose by one-step method[J].Chemical Industry and Engineering Progress,2016,35(2):559-564.
[14]庄森炀,唐丽荣,卢麒麟,等.磷酸锆辅助催化水解菌糠制备纳米纤维素晶体的性能[J].化工进展,2016,35(3):866-871.ZHUANG S Y,TANG L R,LU Q L,et al.Preparation of cellulose nanocrystals by solid catalyst zirconium phosphate assisted hydrolysis from spent mushroom substrate[J].Chemical Industry and Engineering Progress,2016,35(3):866-871.
[15]赵云,陈萧宇,庞勇,等.纳米纤维素增强形状记忆聚氨酯材料的研究[J].塑料工业,2015,43(8):115-118+123.ZHAO Y,CHEN X,PANG Y,et al.Study on cellulose nanocrystals reinforced shape memory polyurethanes[J].China Plastics Industry,2015,43(8):115-118,123.
[16]BIYANI M V,FOSTER E J,WEDER C.Light-healable supramolecular nanocomposites based on modified cellulose nanocrystals[J].ACS Macro Letters,2013,2:236-240.
[17]FOX J,WIE J J,GREENLAND B W,et al.High-strength,healable,supramolecular polymer nanocomposites[J].Journal of the American Chemical Society,2012,134:5362-5368.
[18]COULIBALY S,ROULIN A,BALOG S,et al.Reinforcement of optically healable supramolecular polymers with cellulose nanocrystals[J].Macromolecules,2014,47:152-160.
[19]YANG J,ZHANG X,MA M,et al.Modulation of assembly and dynamics in colloidal hydrogels via ionic bridge from cellulose nanofibrils and poly(ethylene glycol)[J].ACS Macro Letters,2015,4:829-833.
[20]TANG L,ZHUANG S,LU Q,et al.Ultrasonication-assisted preparation of esterified cellulose nanocrystals via one-pot simultaneous reaction[J].Journal of Biobased Materials and Bioenergy,2016,10:27-33.
[21]TANG L,HUANG B,LU Q,et al.Ultrasonication-assisted manufacture of cellulose nanocrystals esterified with acetic acid[J].Bioresource Technology,2013,127:100-105.