【毕业设计精品】核应急废水处理用普鲁士蓝碳纳米管海绵吸附材料及性能.doc
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1、中图分类号:X703.1、 TL942 论文编号:1028706 14-S101学科分类号:082704 硕士学位论文 核应急废水处理用普鲁士蓝/碳纳米管海绵吸附材料及性能研究生姓名学科、专业辐射防护及环境保护研究方向放射性废物处理指导教师南京航空航天大学研究生院 材料科学与技术学院二一四年三月Nanjing University of Aeronautics and AstronauticsThe Graduate SchoolCollege of Materials Science and TechnologyNuclear Emergency Wastewater Treatment w
2、ith Prussian Blue / Carbon Nanotube Sponge Absorbing Material and PerformanceA Thesis inRadiation Protection and Environmental ProtectionbyWuting SHENAdvised byProf. Yaodong DAISubmitted in Partial Fulfillmentof the Requirementsfor the Degree ofMaster of Engineering March, 2014承诺书本人声明所呈交的硕士学位论文是本人在导
3、师指导下进行的研究工作及取得的研究成果。除了文中特别加以标注和致谢的地方外,论文中不包含其他人已经发表或撰写过的研究成果,也不包含为获得南京航空航天大学或其他教育机构的学位或证书而使用过的材料。本人授权南京航空航天大学可以将学位论文的全部或部分内容编入有关数据库进行检索,可以采用影印、缩印或扫描等复制手段保存、汇编学位论文。(保密的学位论文在解密后适用本承诺书) 作者签名: 日 期: 核应急废水处理用普鲁士蓝/碳纳米管海绵吸附材料及性能摘 要全球性的能源危机带来了核能及核技术的蓬勃发展。与此同时,核能行业产生的环境问题逐渐暴露在我们面前,其中核废水的排放和泄露严重影响人们的健康安全和生活环境。
4、因此,大力发展核应急废水处理技术备受重视。常用的放射性废水处理技术是离子交换法,而技术关键在于交换材料的制备。本文利用资源丰富、价格低廉的聚氨酯海绵为模板、以酚醛树脂为炭源,制备了三维开架多孔的碳纳米管海绵。并从中选择最适合炭化温度的海绵作为基底,通过原位生长法将Fe-Fe(II) 、Ni-Fe(II) 和Ni-Fe() 普鲁士蓝连接到碳纳米管海绵上。通过SEM、XRD、残炭率和体积收缩率等表征证明,模板法得到的样品复制了海绵的三维立体孔洞结构,其孔的表面和孔壁分布着大量的碳纳米管。而不同炭化温度的基底对普鲁士蓝的生长有很大影响,400 C为比较理想的炭化温度。通过SEM、IR对三种普鲁士蓝/
5、碳纳米管海绵表征结果表明,普鲁士蓝沿着海绵孔隙表面的碳纳米管生长。利用ICP测试得出Ni-Fe(II)普鲁士蓝含量占Ni-Fe(II)普鲁士蓝/碳纳米管海绵样品的4.63 wt%。本文具体研究了碳纳米管海绵和Ni-Fe(II)普鲁士蓝/碳纳米管海绵对Cu2+的去除率随时间、吸附剂剂量和溶液pH值变化的影响。实验结果表明,相对于纯碳纳米管海绵,Ni-Fe(II)普鲁士蓝/碳纳米管海绵同时兼备了吸附和离子交换性能,但主要表现为离子交换作用。Ni-Fe(II)普鲁士蓝/碳纳米管海绵对Cu2+的去除率随时间的增大而增强,在4 h左右达到平衡。在中性和弱酸性条件下,Ni-Fe(II)普鲁士蓝/碳纳米管海
6、绵去除效果最佳。在室温25 C,pH=6,超声4 h,用量为1 g时,样品对Cu2+最大的吸附容量为9.783 mg/g。Ni-Fe(II)普鲁士蓝/碳纳米管海绵的平衡吸附容量与Cu2+浓度之间的关系符合弗罗因德利希模型。论文研究了Ni-Fe(II)普鲁士蓝/碳纳米管海绵对不同价态离子的选择性。在Ni-Fe(II)普鲁士蓝/碳纳米管海绵在与一价Cs+溶液反应中,Ni-Fe(II)普鲁士蓝中的K+对Cs+进行离子交换;而在与二价和三价的离子溶液反应中,离子交换主要是通过目标离子(Cr3+、Sr2+、Cu2+)与K+和Ni2+发生交换。结合ICP和穆斯堡尔测试得出Ni-Fe(II)普鲁士蓝/碳纳米
7、管海绵对Cs+具有最高的离子选择性,吸附容量达13.46 mg/g。Ni-Fe(II)普鲁士蓝对四种离子选择性顺序为Cs+Sr2+Cr3+Cu2+。关键词:碳纳米管海绵,普鲁士蓝,无机离子交换材料,核应急废水,吸附,离子交换,穆斯堡尔谱ABSTRACTThe growing energy crisis has brought the rapid development of nuclear science and technology. But at the same time, environmental problems of nuclear industry are measuring
8、their exposure to everyone, which can seriously affect peoples health and living environment, particularly the nuclear emergency wastewater. The issue of developing nuclear emergency wastewater treatment technology has caught redoubled attention from various countries in the world.At present, ion ex
9、change is most widely used due to its conveniency and efficiency,and thus material is the key of this method. Here in our work, a novel kind of spongiform adsorbent was synthesized by template replication, using the abundant and cheap polyurethane foam as a template, phenolic resin and multi-walled
10、carbon nanotubes as carbon sources. Then using the optimum sponge as the base, decorated Fe-Fe(II), Ni-Fe(II) and Ni-Fe() Prussian blue onto the carbon nanotube sponge by in situ growth method. SEM, XRD, char yield and volume shrinkage characterization demonstrated that the carbon nanotube sponge wa
11、s equipped with large holes and porous structure, and there was a large number of MWNTs uniformly deposited on the surface and internal cavities. Different carbonization temperature had great influence on the growth of prussian blue nanoparticles, 400 C was proved to be the optimal carbonization. SE
12、M and IR showed that in the prussian-blue/carbon nanotube sponge adsorbent material, prussian blue nanoparticles were fastened on cell walls of carbon nanotube sponge, and the Ni-Fe(II) Prussian blue content of Ni-Fe(II) prussian blue/ carbon nanotube sponge was tested to be 4.63 wt% by ICP.The chan
13、ge of the adsorption rate of Ni-Fe(II) prussian blue/ carbon nanotube sponge for Cu2+ with time, sorbent dose and the pH value was investigated. Results showed that compared to carbon nanotube sponge, Ni-Fe(II) prussian blue/ carbon nanotube sponge had both the adsorption ability and ion exchange of
14、 Cu2+, but mainly for ion exchange . The removal of Cu2+ was found to increase with the time and the adsorption equilibrium would reach in about 4 hours. In neutral and weakly acidic conditions, it had the tallest removal efficiency of Cu2+. Cu2+ maximum adsorption capacity could be 9.783 mg/g under
15、 conditions of room temperature 25 C, weakly acidic, time of 4 h and 1 g of sorbent dose. The Freundlich adsorption model could well represent the adsorption of Cu2+ by both carbon nanotube sponge and Ni-Fe(II) prussian blue/ carbon nanotube sponge.Research on selectivity abitility of Ni-Fe(II) prus
16、sian blue/carbon nanotube sponge in different valence state of ions were studied in this paper. By reaction in Cs+ solution, the ion exchange process was between K+ in Ni-Fe (II) prussian blue/carbon nanotube and Cs+ in solution; In ionic solution reacts with divalent and trivalent, the ion exchange
17、 was mainly through the target ion (Cr3+, Sr2+, Cu2+) with K+ and Ni2+. Combined with ICP and Mossbauer, Ni-Fe(II) prussian blue/carbon nanotube sponge showed the highest selectivity for Cs+ in mixed aqueous solution, and its adsorptive capacity of Cs+ reached 13.46 mg/g. It was found that their sel
18、ectivity activities in sequence are as following respectively: Cs+Sr2+Cr3+Cu2+.Keywords: carbon nanotube sponges, prussian blue, inorganic ion exchange materials, nuclear emergency wastewater, adsorption, ion exchange, mossbauer spectrum目 录第一章 绪论11.1引言11.2 放射性废水的分类与来源11.2.1 放射性废水的分类11.2.2 放射性废水的来源11
19、.2.2.1 核电站11.2.2.2 医院放射科21.2.2.3 核相关部门21.3无机离子交换材料对放射性废水处理进展21.3.1有机离子交换树脂31.3.2多价金属磷酸盐41.3.3普鲁士蓝类化合物41.3.4多价金属(过渡金属)的氧化物和氢氧化物51.3.5铝硅化合物61.3.6新型多孔材料61.4穆斯堡尔谱学及其在普鲁士蓝中的应用91.4.1穆斯堡尔谱学概述101.4.2穆斯堡尔谱学原理及基本参数101.4.2.1穆斯堡尔效应原理101.4.2.2穆斯堡尔谱学基本参数111.4.3穆斯堡尔谱学在普鲁士蓝中的应用121.5课题研究内容及创新点141.5.1课题研究内容141.5.2课题研
20、究创新点15第二章 碳纳米管海绵的制备及表征162.1引言162.2实验内容162.2.1模板的选取162.2.2材料的制备172.2.3材料的表征182. 3结果与分析182.3.1碳纳米管海绵制备及性能表征182.3.2碳纳米管海绵XRD表征212.3.3不同炭化温度的碳纳米管海绵残炭率和体积收缩率表征222.4小结24第三章 普鲁士蓝/碳纳米管海绵的制备及表征253.1引言253.2实验内容253.2.1实验材料及仪器253.2.2实验表征263.3结果与分析263.3.1普鲁士蓝/碳纳米管海绵的扫描电镜表征263.3.2普鲁士蓝/碳纳米管海绵的IR表征273.3.3普鲁士蓝类似物/碳纳
21、米管海绵的穆斯堡尔表征293.3.4 Ni-Fe(II)普鲁士蓝/碳纳米管海绵的ICP表征313.4小结31第四章 Ni-Fe(II)普鲁士蓝/碳纳米管海绵对放射性铜离子的去除324.1 引言324.2实验内容324.2.1实验试剂及设备324.2.2 Cu2+溶液的浓度测定334.2.3静态交换吸附实验334.3结果与分析344.3.1时间对去除率的影响344.3.2 pH值对去除率的影响344.3.3吸附剂剂量对去除率的影响354.3.4吸附等温线364.3.5最大吸附容量374.4 小结38第五章 Ni-Fe(II)普鲁士蓝/碳纳米管海绵的离子选择性及穆斯堡尔谱研究395.1引言395.
22、2实验内容395.2.1实验试剂及设备395.2.2离子选择性实验及分析方法395.3 结果与讨论405.3.1 Ni-Fe(II)普鲁士蓝/碳纳米管海绵吸附不同离子前后的ICP研究405.3.2 Ni-Fe(II)普鲁士蓝/碳纳米管海绵吸附不同离子前后的穆斯堡尔谱研究415.4 结论43第六章 总结与展望446.1总结446.2展望45参考文献47致谢47攻读硕士学位期间发表(录用)论文情况54图表清单图1.1 穆斯堡尔谱学实验装置10图1.2 同质异能移及四极分裂原理图12图1.3 同质异能移与铁的价态和自旋态的关系13图1.4 四极分裂值与铁的价态和自旋态的关系14图2.1 聚氨酯海绵模
23、板的热解图17图2.2 碳纳米管海绵炭化温度曲线18图2.3 碳纳米管海绵制备过程19图2.4 不同炭化温度的碳纳米管海绵孔结构和碳纳米管分布SEM照片20图2.5 不同炭化温度的炭/碳纳米管孔结构XRD图谱21图2.6 不同炭化温度下残炭率和体积收缩率的变化22图2.7(a)原始海绵的扫描电镜照片;(b)-(f)碳纳米管海绵(400C)整体和孔壁局部放大照片23图3.1 (a)普鲁士蓝/碳纳米管海绵扫描电镜照片;(b)-(d) 碳纳米管海绵表面修饰Fe-Fe(II) 、Ni-Fe(II)和Ni-Fe()普鲁士蓝扫描电镜照片26图3.2 Fe-Fe(II)普鲁士蓝/碳纳米管海绵红外图谱28图3
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