多級結(jié)構(gòu)石墨烯—羥基磷灰石雜化材料制備及其應(yīng)用研究
發(fā)布時間：2018-10-05 21:33
【摘要】：石墨烯(Graphene)作為新興的二維材料,具有優(yōu)異的電性能、導(dǎo)熱性能、機械性能、極大的表面積,在光電材料、有機染料的吸附和生物醫(yī)學(xué)等領(lǐng)域受到廣泛的關(guān)注和研究。然而,石墨烯的片層之間存在很強的范德華力,導(dǎo)致石墨烯易團聚,很難以單片層穩(wěn)定存在,在與聚合物共混時,難以均勻分散;此外,石墨烯本身缺乏特定的生物活性,這些問題在一定程度上限制了石墨烯在納米復(fù)合材料和生物醫(yī)學(xué)的運用。羥基磷灰石(HA)作為一種天然的無機鹽,主要存在于動物的骨結(jié)構(gòu)中。有難溶于水、生物可降解及骨誘導(dǎo)等優(yōu)點。HA作為吸附劑以及生物醫(yī)用材料都有廣泛的應(yīng)用,但是納米HA易團聚、脆性大、裂韌性差等缺點限制了其實際運用。聚乳酸作為一種重要的生物高分子材料,在組織工程中具有重要應(yīng)用;但是聚乳酸其機械強度較低、韌性差、結(jié)晶速率較低。一種理想的骨組織工程支架材料,其不僅需具有良好的骨傳導(dǎo)性和骨誘導(dǎo)性,而且必須具有良好的生物相容性和機械強度及可塑性。圍繞上述問題,本論文主要開展了以下研究:1.堿性條件下,在氧化石墨烯片層表面原位生長納米羥基磷灰石,可以實現(xiàn)原位還原氧化石墨烯,獲得石墨烯-羥基磷灰石(RGO-HA)雜化材料,負載的羥基磷灰石能夠有效抑制石墨烯片層之間的π-πstacking作用,實現(xiàn)還原氧化石墨烯和羥基磷灰石的協(xié)同分散。使用紅外光譜(FT-IR)、透射電鏡(TEM)、X射線衍射(XRD)、X射線電子能譜分析(XPS)、拉曼光譜等測試表征RGO-HA雜化材料。RGO-HA雜化材料作為吸附劑,進行吸附動力學(xué)、等溫吸附和pH值對吸附的影響研究。實驗結(jié)果表明:1、RGO-HA對有機染料的吸附過程包含物理吸附和化學(xué)吸附;2、RGO-HA吸附劑表層吸附位點吸附能力相同且分布均勻;3、RGO-HA吸附劑更適用于陽離子有機染料的吸附,在堿性條件下吸附能力呈現(xiàn)急劇上升趨勢。2.先制備表面接枝聚(右旋乳酸)的RGO-HA(RGO-HA-g-PDLA),再通過靜電紡絲技術(shù)制備載有辛伐他汀(SIM)的RGO-HA-g-PDLA/PLLA復(fù)合納米纖維支架材。將制備的含有辛伐他汀(SIM)的RGO-HA-g-PDLA/PLLA的納米纖維膜按照SIM濃度由高向低卷成圓柱狀,接著吸附I型膠原、并利用戊二醛溶液作為交聯(lián)劑,對支架材料進行交聯(lián),最后將其切成薄片支架材料植入雄性BALB/c小鼠顱骨進行修復(fù)。體外礦化實驗結(jié)果表明制備的RGO-HA-g-PDLA/PLLA@SIM支架材料相對于PLLA、PLLA@SIM和RGO-HA-g-PDLA/PLLA具有更好的鈣沉積能力。體外藥物釋放結(jié)果表明RGO-HA-g-PDLA/PLLA纖維膜中的SIM有效釋放時間高達30天,相對于PLLA支架材料有更持久有效的釋放,SIM的釋放量高達88%,顱骨的修復(fù)實驗結(jié)果表明RGO-HA-g-PDLA/PLLA@SIM支架材料具有更強的促進骨組織修復(fù)能力。
[Abstract]:Graphene (Graphene), as a new two-dimensional material, has been widely studied in the fields of optoelectronic materials, adsorption of organic dyes and biomedicine due to its excellent electrical properties, thermal conductivity, mechanical properties and great surface area. However, there is a strong van der Waals force between the layers of graphene, which leads to easy agglomeration of graphene, which makes it difficult for monolayer to exist stably and is difficult to disperse uniformly when mixed with polymer. In addition, graphene itself lacks specific biological activity. These problems limit the application of graphene in nanocomposites and biomedicine to some extent. Hydroxyapatite (HA), as a natural inorganic salt, mainly exists in the bone structure of animals. Ha is widely used as adsorbent and biomedical material in water, biodegradability and bone induction. However, nano-sized HA is easy to agglomerate, brittle and poor fracture toughness, which limits its practical application. Polylactic acid (PLA), as an important biomaterial, has important applications in tissue engineering, but its mechanical strength, toughness and crystallization rate are low. An ideal scaffold for bone tissue engineering should not only have good bone conductivity and bone induction, but also have good biocompatibility, mechanical strength and plasticity. Around the above question, this thesis mainly carried out the following research: 1. Nano-hydroxyapatite was grown on the surface of graphene oxide in situ under alkaline condition. In situ reduction of graphene and hydroxyapatite (RGO-HA) hybrid material could be achieved. The supported hydroxyapatite can effectively inhibit the 蟺-蟺 stacking interaction between the graphene lamellae and realize the synergistic dispersion of reduced graphene and hydroxyapatite. The adsorption kinetics, isothermal adsorption and the effect of pH value on the adsorption of RGO-HA hybrid material. RGO-HA hybrid material were characterized by infrared spectroscopy (FT-IR), transmission electron microscopy (TEM) (TEM) X-ray diffraction (XRD) X-ray electron spectroscopy (XRD) and Raman spectroscopy (XPS),). The adsorption kinetics, isothermal adsorption and the effect of pH value on the adsorption were studied. The experimental results show that the adsorption process of organic dyes by RGO-HA includes physical adsorption and chemical adsorption. The adsorption ability of RGO-HA on the surface layer of RGO-HA is the same, and the RGO-HA adsorbent is more suitable for the adsorption of cationic organic dyes. The adsorption capacity showed a sharp upward trend under alkaline conditions. Surface grafted RGO-HA (RGO-HA-g-PDLA) was prepared, and then RGO-HA-g-PDLA/PLLA composite nanofiber scaffold containing simvastatin (SIM) was prepared by electrostatic spinning. The prepared RGO-HA-g-PDLA/PLLA nanofiber membrane containing simvastatin (SIM) was rolled into columns according to the concentration of SIM from high to low. Then collagen I was adsorbed, and glutaraldehyde solution was used as crosslinking agent to cross-link the scaffold. Finally, a thin slice of the scaffold was implanted into the skull of male BALB/c mice for repair. The results of in vitro mineralization test showed that the prepared RGO-HA-g-PDLA/PLLA@SIM scaffold had better calcium deposition ability than that of PLLA,PLLA@SIM and RGO-HA-g-PDLA/PLLA. The results of drug release in vitro showed that the effective release time of SIM in RGO-HA-g-PDLA/PLLA fiber membrane was up to 30 days. Compared with PLLA scaffold material, the release amount of SIM was as high as 88%. The results of skull repair experiment showed that RGO-HA-g-PDLA/PLLA@SIM scaffold material had a stronger ability to promote bone tissue repair.
【學(xué)位授予單位】：南昌大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TB332
本文編號：2254941
[Abstract]:Graphene (Graphene), as a new two-dimensional material, has been widely studied in the fields of optoelectronic materials, adsorption of organic dyes and biomedicine due to its excellent electrical properties, thermal conductivity, mechanical properties and great surface area. However, there is a strong van der Waals force between the layers of graphene, which leads to easy agglomeration of graphene, which makes it difficult for monolayer to exist stably and is difficult to disperse uniformly when mixed with polymer. In addition, graphene itself lacks specific biological activity. These problems limit the application of graphene in nanocomposites and biomedicine to some extent. Hydroxyapatite (HA), as a natural inorganic salt, mainly exists in the bone structure of animals. Ha is widely used as adsorbent and biomedical material in water, biodegradability and bone induction. However, nano-sized HA is easy to agglomerate, brittle and poor fracture toughness, which limits its practical application. Polylactic acid (PLA), as an important biomaterial, has important applications in tissue engineering, but its mechanical strength, toughness and crystallization rate are low. An ideal scaffold for bone tissue engineering should not only have good bone conductivity and bone induction, but also have good biocompatibility, mechanical strength and plasticity. Around the above question, this thesis mainly carried out the following research: 1. Nano-hydroxyapatite was grown on the surface of graphene oxide in situ under alkaline condition. In situ reduction of graphene and hydroxyapatite (RGO-HA) hybrid material could be achieved. The supported hydroxyapatite can effectively inhibit the 蟺-蟺 stacking interaction between the graphene lamellae and realize the synergistic dispersion of reduced graphene and hydroxyapatite. The adsorption kinetics, isothermal adsorption and the effect of pH value on the adsorption of RGO-HA hybrid material. RGO-HA hybrid material were characterized by infrared spectroscopy (FT-IR), transmission electron microscopy (TEM) (TEM) X-ray diffraction (XRD) X-ray electron spectroscopy (XRD) and Raman spectroscopy (XPS),). The adsorption kinetics, isothermal adsorption and the effect of pH value on the adsorption were studied. The experimental results show that the adsorption process of organic dyes by RGO-HA includes physical adsorption and chemical adsorption. The adsorption ability of RGO-HA on the surface layer of RGO-HA is the same, and the RGO-HA adsorbent is more suitable for the adsorption of cationic organic dyes. The adsorption capacity showed a sharp upward trend under alkaline conditions. Surface grafted RGO-HA (RGO-HA-g-PDLA) was prepared, and then RGO-HA-g-PDLA/PLLA composite nanofiber scaffold containing simvastatin (SIM) was prepared by electrostatic spinning. The prepared RGO-HA-g-PDLA/PLLA nanofiber membrane containing simvastatin (SIM) was rolled into columns according to the concentration of SIM from high to low. Then collagen I was adsorbed, and glutaraldehyde solution was used as crosslinking agent to cross-link the scaffold. Finally, a thin slice of the scaffold was implanted into the skull of male BALB/c mice for repair. The results of in vitro mineralization test showed that the prepared RGO-HA-g-PDLA/PLLA@SIM scaffold had better calcium deposition ability than that of PLLA,PLLA@SIM and RGO-HA-g-PDLA/PLLA. The results of drug release in vitro showed that the effective release time of SIM in RGO-HA-g-PDLA/PLLA fiber membrane was up to 30 days. Compared with PLLA scaffold material, the release amount of SIM was as high as 88%. The results of skull repair experiment showed that RGO-HA-g-PDLA/PLLA@SIM scaffold material had a stronger ability to promote bone tissue repair.
【學(xué)位授予單位】：南昌大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TB332
【參考文獻】
相關(guān)期刊論文 前1條
1 江國棟;常青;楊福福;胡曉允;唐和清;;超聲輔助合成磁性四氧化三鐵/氧化石墨烯復(fù)合物及其在染料去除中的應(yīng)用（英文）[J];Chinese Journal of Chemical Engineering;2015年03期
，本文編號：2254941
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