多級復(fù)合孔復(fù)雜中空結(jié)構(gòu)的可控合成及其構(gòu)效關(guān)系
發(fā)布時間：2018-11-05 08:17
【摘要】：本文主要合成了三種不同材料的具有多級復(fù)合孔的復(fù)雜中空結(jié)構(gòu),即多殼或多核結(jié)構(gòu)。由于結(jié)構(gòu)上的特殊性和性能上的優(yōu)越性,具有不同內(nèi)部核殼結(jié)構(gòu)的微納米材料越來越多地受到人們的關(guān)注。這種結(jié)構(gòu)的材料通常具有較低的密度,較大的比表面積,較高的負(fù)載量和催化效率,并且可以有效地縮短物質(zhì)或電荷傳輸過程的路徑,因而在微尺度反應(yīng)器、藥物載體等許多領(lǐng)域都有重要的應(yīng)用前景。然而目前來說,對于具有復(fù)雜內(nèi)部核殼結(jié)構(gòu)的中空微納米材料的可控合成仍然是一大挑戰(zhàn)。另一方面,一種新型的多孔材料——多級復(fù)合孔材料,隨著多孔材料的發(fā)展而逐漸產(chǎn)生。它不同于單一孔徑的多孔材料,這種復(fù)合孔材料具有兩種或兩種以上不同孔徑的孔結(jié)構(gòu),并且按孔徑逐級分布。這樣的結(jié)構(gòu)既可以保證產(chǎn)物有較大的比表面積和活性位點(diǎn),又有助于物質(zhì)的傳遞,減少物質(zhì)擴(kuò)散過程中所受到的阻力。故而它的各方面性能優(yōu)越,逐漸受到研究者的青睞。但是同時具備多級復(fù)合孔和不同內(nèi)部核殼結(jié)構(gòu)的微納米材料尚未見報道。本論文基于目前的研究現(xiàn)狀和研究趨勢,以合成同時具有多級復(fù)合孔和多殼或多核內(nèi)部結(jié)構(gòu)的微納米材料為研究目標(biāo),著重利用模板法合成具有多級復(fù)合孔的多殼/核結(jié)構(gòu)的微納米材料,對產(chǎn)物用X-射線衍射(XRD)、掃描電鏡(SEM)、透射電鏡(TEM)、掃描透射電鏡(STEM)等手段進(jìn)行表征,并探討它們在相關(guān)應(yīng)用方面的性能。進(jìn)一步地,我們對產(chǎn)物的生成機(jī)理進(jìn)行了闡述,以此指導(dǎo)其他類似結(jié)構(gòu)產(chǎn)物的合成,為其他材料的合成提供借鑒。本論文主要開展了以下幾項工作:(1)可控合成了具有多級復(fù)合孔的不同殼層的Zn O中空材料,并研究了其形成機(jī)理和光催化性能。采用簡化模板法,分別可控合成了具有多級復(fù)合孔的單層、雙層和三層的Zn O中空材料。通過對產(chǎn)物的表征,確定了它們的大小、形貌及內(nèi)部結(jié)構(gòu);通過對合成過程的實(shí)時監(jiān)測,提出了溫度梯度形成機(jī)理;并研究了產(chǎn)物在光催化方面的性能,表明隨著殼層數(shù)的增加,Zn O對Rh B的催化降解性能和催化劑的循環(huán)效率都隨之提高,在水處理方面表現(xiàn)出良好的應(yīng)用前景。尤其是產(chǎn)物形成機(jī)理的研究,有助于指導(dǎo)類似結(jié)構(gòu)產(chǎn)物的合成,從而更好的控制合成具有不同內(nèi)部結(jié)構(gòu)的中空微納米材料。(2)可控合成了具有多級復(fù)合孔結(jié)構(gòu)的多殼Ca CO3中空材料,并分析了產(chǎn)物的形成機(jī)理。我們巧妙利用有機(jī)酸鈣的熱分解,并通過對反應(yīng)條件的調(diào)整,實(shí)現(xiàn)了對產(chǎn)物形貌的有效調(diào)控,得到了具有多級復(fù)合孔結(jié)構(gòu)的單層、雙層和三層Ca CO3中空材料。采用多種測試手段對樣品進(jìn)行表征分析,確定了產(chǎn)物的相關(guān)結(jié)構(gòu)及性質(zhì);通過對反應(yīng)過程的監(jiān)測和分析,我們認(rèn)為不同結(jié)構(gòu)產(chǎn)物的形成依賴于模板層層加熱機(jī)理。多層Ca CO3屬于氧化物之外的多層殼材料,豐富了多層殼材料的種類,為其他類似結(jié)構(gòu)碳酸鹽材料的合成提供了借鑒。(3)探討了所合成的具有多級復(fù)合孔的三層結(jié)構(gòu)碳酸鈣(記為HPTHMs)在作為p H響應(yīng)性抗癌藥物載體方面的性能。我們將HPTHMs應(yīng)用于抗癌藥物鹽酸阿霉素(DOX-HCl)的負(fù)載和不同p H條件下的釋放實(shí)驗。結(jié)果表明,HPTHMs作為藥物載體,具有較高的藥物吸附效率和負(fù)載量,并且對藥物呈現(xiàn)良好的p H響應(yīng)性釋放;通過流式細(xì)胞術(shù)(FCM)、激光共聚焦顯微分析(CLSM)等手段證明了載體的存在,提高了癌細(xì)胞對DOX的攝入,增強(qiáng)了抗癌效果;體內(nèi)/外實(shí)驗進(jìn)一步證明載藥后的HPTHMs-DOX樣品對癌細(xì)胞和腫瘤組織的生長都有較好的抑制作用。可以看到,HPTHMs在響應(yīng)性抗癌藥物運(yùn)輸方面具有良好的應(yīng)用前景。(4)合成了具有多級復(fù)合孔的多核結(jié)構(gòu)La2O2CO3材料,并初步探討了產(chǎn)物的生成機(jī)理。采用模板法,并利用醋酸鑭鹽的熱分解,得到了具有多級復(fù)合孔和不同核數(shù)的多核結(jié)構(gòu)La2O2CO3材料。通過一系列的表征觀察了產(chǎn)物的形貌及多孔結(jié)構(gòu);并通過中間產(chǎn)物的存在對其形成機(jī)理進(jìn)行了初步探討,當(dāng)然確切的機(jī)理仍需要更多的實(shí)驗數(shù)據(jù)證明。多孔以及多核結(jié)構(gòu)的存在,有利于La2O2CO3與磷酸鹽的接觸,提高對磷酸鹽的沉淀效率,為其作為高效的磷酸鹽結(jié)合劑提供可能。
[Abstract]:In this paper, three complex hollow structures with multi-stage composite pores, i.e. multi-shell or multi-core structures, are synthesized. Due to the particularity and superiority of structure, micro-materials with different internal core shell structures have been paid more and more attention. The material of this structure usually has lower density, larger specific surface area, higher loading and catalytic efficiency, and can effectively shorten the path of substance or charge transfer process, and has important application prospect in many fields such as micro-scale reactor and drug carrier. At present, however, the controllable synthesis of hollow micro-materials with complex internal core shell structures remains a challenge. On the other hand, a new porous material _ multi-stage composite pore material is gradually developed with the development of porous material. which is different from the porous material of a single pore size, and the composite pore material has two or more pore structures with different pore sizes, and is distributed in a step by step according to the pore size. Such a structure can ensure that the product has a larger specific surface area and an active site, but also contributes to the transfer of substances and reduces the resistance to substance diffusion. So its aspects are superior and gradually favored by researchers. However, micro-materials with multi-stage composite pores and different internal core shell structures have not been reported. Based on current research situation and trend of research, this paper aims at synthesizing micro-nano material with multi-stage composite pore and multi-shell or multi-core internal structure at the same time, and mainly uses template method to synthesize micro-nano material with multi-shell/ core structure with multi-stage composite pores, The products were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), scanning electron microscope (STEM), etc. Further, we set forth the mechanism of product formation, so as to guide the synthesis of other similar structure products and provide reference for the synthesis of other materials. The paper mainly carries out the following work: (1) Controllable synthesis of Zn O hollow materials with different shell layers with multi-stage composite pores, and studies its formation mechanism and photocatalytic performance. By adopting the simplified template method, a single layer, a double layer and a three-layer Zn O hollow material with a multi-stage composite pore are respectively controlled and synthesized. Through the characterization of the product, the size, morphology and internal structure of the product are determined. Through real-time monitoring of the synthesis process, the forming mechanism of the temperature gradient is put forward, and the performance of the product in photocatalysis is studied, indicating that with the increase of the number of layers of the shell, The catalytic degradation performance of the Zn O to Rh B and the cycle efficiency of the catalyst are improved, and a good application prospect is shown in the water treatment. In particular, the research on the formation mechanism of products helps to guide the synthesis of similar structural products, so as to better control the synthesis of hollow micro-materials with different internal structures. (2) a multi-shell Ca-CO3 hollow material with multi-stage composite pore structure is synthesized and the formation mechanism of the product is analyzed. We skillfully utilize the thermal decomposition of organic acid calcium, and through the adjustment of the reaction conditions, the effective regulation of the product morphology is realized, and a single layer, a double layer and a three-layer Ca CO3 hollow material with a multi-stage composite pore structure are obtained. The structure and properties of the product are determined by means of a variety of test methods. Through the monitoring and analysis of the reaction process, we believe that the formation of different structural products depends on the heating mechanism of the template layer. The multi-layer CaCO3 belongs to the multi-layer shell material other than the oxide, enriches the variety of the multi-layer shell material and provides a reference for the synthesis of other similar structural carbonate materials. (3) The properties of the synthesized three-layer structure calcium carbonate (HPTHMs) with multi-stage composite pore were discussed. We applied HPTHMs to the loading of anti-cancer drug hydrochloride (DOX-HCl) and release experiments under different p-H conditions. The results show that HPTHMs can be used as drug carrier, have higher drug adsorption efficiency and loading capacity, and have good p-H response release on drug; by flow cytometry (FCM) and laser confocal microscopy (CLSM), the existence of vector is proved. The uptake of DOX by cancer cells is improved, and the anti-cancer effect is enhanced; and in vivo/ external experiments further prove that the HPTHMs-DOX sample after drug loading has good inhibiting effect on the growth of cancer cells and tumor tissues. It can be seen that HPTHMs have good application prospects in response to anti-cancer drug transport. (4) The multi-core La2O2CO3 material with multi-stage composite pores was synthesized, and the product formation mechanism was preliminarily discussed. A multi-core La2O2CO3 material with multi-stage composite pores and different cores was obtained by using template method and thermal decomposition of zinc acetate salt. The morphology and porous structure of the product are observed through a series of characterization, and the formation mechanism of the product is preliminarily discussed through the presence of intermediate products. The existence of porous and multi-core structures facilitates the contact of La2O2CO3 with phosphate, improves the precipitation efficiency of phosphate, and provides it as a high-efficiency phosphate binding agent.
【學(xué)位授予單位】：河南師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TB383.4
本文編號：2311476
[Abstract]:In this paper, three complex hollow structures with multi-stage composite pores, i.e. multi-shell or multi-core structures, are synthesized. Due to the particularity and superiority of structure, micro-materials with different internal core shell structures have been paid more and more attention. The material of this structure usually has lower density, larger specific surface area, higher loading and catalytic efficiency, and can effectively shorten the path of substance or charge transfer process, and has important application prospect in many fields such as micro-scale reactor and drug carrier. At present, however, the controllable synthesis of hollow micro-materials with complex internal core shell structures remains a challenge. On the other hand, a new porous material _ multi-stage composite pore material is gradually developed with the development of porous material. which is different from the porous material of a single pore size, and the composite pore material has two or more pore structures with different pore sizes, and is distributed in a step by step according to the pore size. Such a structure can ensure that the product has a larger specific surface area and an active site, but also contributes to the transfer of substances and reduces the resistance to substance diffusion. So its aspects are superior and gradually favored by researchers. However, micro-materials with multi-stage composite pores and different internal core shell structures have not been reported. Based on current research situation and trend of research, this paper aims at synthesizing micro-nano material with multi-stage composite pore and multi-shell or multi-core internal structure at the same time, and mainly uses template method to synthesize micro-nano material with multi-shell/ core structure with multi-stage composite pores, The products were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), scanning electron microscope (STEM), etc. Further, we set forth the mechanism of product formation, so as to guide the synthesis of other similar structure products and provide reference for the synthesis of other materials. The paper mainly carries out the following work: (1) Controllable synthesis of Zn O hollow materials with different shell layers with multi-stage composite pores, and studies its formation mechanism and photocatalytic performance. By adopting the simplified template method, a single layer, a double layer and a three-layer Zn O hollow material with a multi-stage composite pore are respectively controlled and synthesized. Through the characterization of the product, the size, morphology and internal structure of the product are determined. Through real-time monitoring of the synthesis process, the forming mechanism of the temperature gradient is put forward, and the performance of the product in photocatalysis is studied, indicating that with the increase of the number of layers of the shell, The catalytic degradation performance of the Zn O to Rh B and the cycle efficiency of the catalyst are improved, and a good application prospect is shown in the water treatment. In particular, the research on the formation mechanism of products helps to guide the synthesis of similar structural products, so as to better control the synthesis of hollow micro-materials with different internal structures. (2) a multi-shell Ca-CO3 hollow material with multi-stage composite pore structure is synthesized and the formation mechanism of the product is analyzed. We skillfully utilize the thermal decomposition of organic acid calcium, and through the adjustment of the reaction conditions, the effective regulation of the product morphology is realized, and a single layer, a double layer and a three-layer Ca CO3 hollow material with a multi-stage composite pore structure are obtained. The structure and properties of the product are determined by means of a variety of test methods. Through the monitoring and analysis of the reaction process, we believe that the formation of different structural products depends on the heating mechanism of the template layer. The multi-layer CaCO3 belongs to the multi-layer shell material other than the oxide, enriches the variety of the multi-layer shell material and provides a reference for the synthesis of other similar structural carbonate materials. (3) The properties of the synthesized three-layer structure calcium carbonate (HPTHMs) with multi-stage composite pore were discussed. We applied HPTHMs to the loading of anti-cancer drug hydrochloride (DOX-HCl) and release experiments under different p-H conditions. The results show that HPTHMs can be used as drug carrier, have higher drug adsorption efficiency and loading capacity, and have good p-H response release on drug; by flow cytometry (FCM) and laser confocal microscopy (CLSM), the existence of vector is proved. The uptake of DOX by cancer cells is improved, and the anti-cancer effect is enhanced; and in vivo/ external experiments further prove that the HPTHMs-DOX sample after drug loading has good inhibiting effect on the growth of cancer cells and tumor tissues. It can be seen that HPTHMs have good application prospects in response to anti-cancer drug transport. (4) The multi-core La2O2CO3 material with multi-stage composite pores was synthesized, and the product formation mechanism was preliminarily discussed. A multi-core La2O2CO3 material with multi-stage composite pores and different cores was obtained by using template method and thermal decomposition of zinc acetate salt. The morphology and porous structure of the product are observed through a series of characterization, and the formation mechanism of the product is preliminarily discussed through the presence of intermediate products. The existence of porous and multi-core structures facilitates the contact of La2O2CO3 with phosphate, improves the precipitation efficiency of phosphate, and provides it as a high-efficiency phosphate binding agent.
【學(xué)位授予單位】：河南師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TB383.4
【共引文獻(xiàn)】
相關(guān)期刊論文 前1條
1 劉軍;黃春艷;賀全國;;磁性鐵氧化物納米粒子在藥劑學(xué)上的應(yīng)用[J];化學(xué)通報;2014年01期
相關(guān)博士學(xué)位論文 前2條
1 陳帥君;葉酸受體介導(dǎo)的載順鉑磁性納米pH敏感靶向給藥系統(tǒng)研究[D];南方醫(yī)科大學(xué);2013年
2 劉永軍;基于診斷治療學(xué)多功能納米系統(tǒng)用于肝細(xì)胞癌的分子診斷與治療[D];山東大學(xué);2014年
相關(guān)碩士學(xué)位論文 前3條
1 于川茗;硫酸軟骨素基聚合物膠束的制備及其性能研究[D];蘭州大學(xué);2014年
2 劉軍;復(fù)合空心磁性納米粒子的制備、表征與藥物輸運(yùn)應(yīng)用[D];湖南工業(yè)大學(xué);2014年
3 劉文;K5多糖—阿霉素綴合物的制備及其藥物傳遞性能研究[D];江南大學(xué);2014年
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