密级:
硕士学位论文
作者姓名：万林林自动钎焊设备
指导教师：黄爱生研究员
激光切割烟雾净化器
中国科学院宁波材料技术与工程研究所学位类别：理学硕士学科专业：有机化学
研究所：中国科学院宁波材料技术与工程研究所
光触媒仿真花二零一七年五月养蜂专用车
Study on the Synthesis and application of UiO-66-NH2
By
Linlin Wan
A Dissertation Submitted to
University of Chinese Academy of Sciences
In partial fulfillment of the requirement
For the degree of
Master of Natural Science
Ningbo Institute of Materials Technology&Engineering, Chinese Academy of Sciences
May,2017
摘要
摘要
金属有机框架材料(Metal Organic Frameworks,MOFs)是近几十年来迅猛发展的一类材料，它是由金
属团簇和有机配体通过配位键自组装而成的一类三维多孔晶体化合物。MOFs材料具有固定孔隙、高结晶度、高比表面积、优良的可调节性和功能化性能，使得其在气体吸附，催化，药物传输和传感器方面有巨大的应用潜力。但由于现存的大多数MOFs材料稳定性不高，使得其在工业上的应用受到限制。因此，要实现MOFs在工业中的应用，一方面要提高材料的稳定性。另一方面，要开展更合适的合成方法来制备低能耗的MOFs材料。
UiO-66材料的水热稳定性，化学稳定性及耐湿性好，因此其在液体分离或是气体分离应用方面引起了研究人员的极大兴趣。本论文以UiO-66-NH2为研究对象，系统性的考察了UiO-66-NH2微波合成，考察了微波合成UiO-66-NH2晶体分别在273K和293K条件下对CO2的吸附容量。并研究了UiO-66-NH2的膜制备过程，对合成的膜材料进行了海水渗透汽化测试。本论文的具体工作如下：（1）分别采用溶剂热合成法及微波辅助加热法，选用四氯化锆作为金属源和对苯二甲酸/2-二氨基对苯二甲酸做配体，DMF作溶剂，盐酸作结晶剂，乙酸作为调制剂，在设定温度下反应，得到产物UiO-66-NH2。 （2）采用粉末X-射线衍射，场发射扫描电镜，热重分析，红外光谱，气体吸附等表征手段对合成的晶体材料进行物理化学性能表征。结果显示，可以在微波条件下迅速合成晶体形貌完美的UiO-66-NH2晶体颗粒。对所获产品进行气体吸脱附测试，结果表明UiO-66-NH2在CO2捕获方面有着良好的应用价值。
（3）采用原位溶剂热法在APTES（3-氨丙基三乙氧基硅烷）修饰的多孔氧化铝基底上制备出尺寸均一的UiO-66-NH2膜，并对制备的UiO-66-NH2膜通过渗透汽化实现海水淡化。
微波辅助合成主要研究了微波辐射时间，温度，调制剂浓度对UiO-66-NH2形貌，结晶性的影响。由于氨基与CO2间的桥联作用，UiO-66-NH2对CO2的吸附量高达5.75mmol/g，并且在298K下对CO2/N2的理想分离因子达到66。对制备的UiO-66-NH2进行海水淡化测试，测试结果显示UiO-66-NH2膜对3.5wt%的海水具有很好的分离性能，在348K条件下的盐离子截留率都在99.97%以上。
关键词：UiO-66-NH2合成，微波辅助加热，CO2吸附，UiO-66-NH2膜，海水淡化，渗透汽化
I
吸音墙
Abstract
Abstract
电极箔
Metal-organic frameworks(MOFs)are a series of emerging materials developed in recent decades，which consist of metallic nodes joined in an ordered fashion by organic linker molecules to generate a3-D porous crystal compound.Due to their specific nature including permanent porosity,high crystallinity,high surface areas, excellent tunability of pore size,crystal shape,and functionality,they ar
e extensively investigated in a wide variety of potential applications in gas adsorption and storage, catalysis,drug delivery,sensors etc.However,the applications of the most existing MOFs materials in industry are limited for their low stability.Indeed,to bring MOFs into an industrial application,on the one hand,their stability must be improved;on the other hand,a vigorous road has to be developed for the reliable and cost-effective synthesis of MOFs。
Attributing to the high hydrothermal and chemical stability of UiO-66, especially its high resistance towards humidity,UiO-66has been drawn much interest for many practical applications in liquid separation and gas separation.This work is a systematic investigation of the microwave-assisted synthesis of UiO-66-NH2.In a detailed study,the influence of microwave irradiation time,temperature,and modulator concentrations on morphology,crystallinity and stability of UiO-66-NH2is investigated with the aim to develop a reliable and reproducible strategy for the preparation of well-shaped UiO-66-NH2.Then the microwave assisted synthesized UiO-66-NH2was test under273K and298K condition for CO2capture.The preparation process of UiO-66-NH2membrane was investigated,and the membrane was tested by pervaporation.The specific work of this paper is as follows:
(1)Solvothermal and microwave assisted heating method were applied for the preparation of UiO-66
and UiO-66-NH2.Zirconium chloride acts as the metal source, terephthalic acid/2-aminoterephthalic acid acts as ligand,and HAc and HCl were used as modulators in different concentrations.The powers(UiO-66-NH2)were obtained after the reaction under specific temperature.
(2)The resulting UiO-66-NH2was characterized by Fourier transform infrared
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