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- 2013
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Copper ferrocyanide are well-known for selective and efficient adsorption of cesium. In this study, copper ferrocyanide on amine-functionalized mesoporous silica(CuFC-EDA-GlyHMS, CuFC-AAHMS) was prepared for removing cesium.
Physicochemical properties of the synthetic adsorbents were characterized by x-ray diffraction(XRD), transmission electron microscopy(TEM), scanning electron microscopy(SEM), FT-IR spectroscopy, elemental analysis and N2 porosimetry.
The adsorption kinetic model were applied to describe the cesium sorption mechanism of CuFC-EDA-GlyHMS and CuFC-AAHMS. Behavior of CuFC-EDA-GlyHMS could be well described by pseudo-second-order kinetic model(PSOM) and behavior of CuFC-AAHMS could be described by Elvoich kinetic model. Most amount of the cesium was adsorbed on the prepared CuFC-EDA-GlyHMS less than 6hr but CuFC-AAHMS adsorbed most amount of the cesium less than 12hr.
Sorption isotherm models were applied to describe the cesium sorption of CuFC-EDA-GlyHMS and CuFC-AAHMS. In Langmuir isotherm model, 17, 30, 50 wt% CuFC-EDA-GlyHMS showed high adsorption affinity to cesium with their capacity of 0.4164 mmol/g, 0.8380 mmol/g, 0.9830 mmol/g and 17, 30 wt% CuFC-AAHMS showed high adsorption affinity to cesium with their capacity of 0.6613 mmol/g, 0.9188 mmol/g.
The effect of co-exisiting cations on the sortpion of cesium onto CuFC-EDA-GlyHMS and CuFC-AAHMS have been investigated. For CuFC-EDA-GlyHMS and CuFC-AAHMS composites, the cesium sorption was negligible in the presence of Na+ and Ca2+. It means that CuFC-EDA-GlyHMS and CuFC-AAHMS composites have cesium selectivity regardless of in the presence of the co-exitsitng cations.
Through thermodynamics studies, for CuFC-EDA-GlyHMS, cesium sorption occur by an endothermic process. All the sorption processes are spontaneous in nature according to the negative values of △G. For CuFC-AAHMS, cesium sorption occur by an endorhermic process and △H value for cesium indicates chemical sorption. All the sorption processes are spontaneous in nature according th the negative values of △G.
As a result, the two types of sorbents are combined in the synthesis method of the co-condensation. The co-condensation has stronger coherence of functional group than grafting. Thus, the co-condensation prevents copper ferrocyanide, which is combined with the sorbent, from leaching. CuFC-EDA-GlyHMS has mesoporous and a large surface area. Its equilibrium velocity is shorter than CuFC-AAHMS. To synthesize CuFC-AAHMS takes shorter time than to synthesize CuFC-EDA-GlyHMS. Also, CuFC-AAHMS has hight adsorption capacity to cesium.
These results make it possible to apply the developed materials for the selective removal of cesium in LIRW in practice.
Physicochemical properties of the synthetic adsorbents were characterized by x-ray diffraction(XRD), transmission electron microscopy(TEM), scanning electron microscopy(SEM), FT-IR spectroscopy, elemental analysis and N2 porosimetry.
The adsorption kinetic model were applied to describe the cesium sorption mechanism of CuFC-EDA-GlyHMS and CuFC-AAHMS. Behavior of CuFC-EDA-GlyHMS could be well described by pseudo-second-order kinetic model(PSOM) and behavior of CuFC-AAHMS could be described by Elvoich kinetic model. Most amount of the cesium was adsorbed on the prepared CuFC-EDA-GlyHMS less than 6hr but CuFC-AAHMS adsorbed most amount of the cesium less than 12hr.
Sorption isotherm models were applied to describe the cesium sorption of CuFC-EDA-GlyHMS and CuFC-AAHMS. In Langmuir isotherm model, 17, 30, 50 wt% CuFC-EDA-GlyHMS showed high adsorption affinity to cesium with their capacity of 0.4164 mmol/g, 0.8380 mmol/g, 0.9830 mmol/g and 17, 30 wt% CuFC-AAHMS showed high adsorption affinity to cesium with their capacity of 0.6613 mmol/g, 0.9188 mmol/g.
The effect of co-exisiting cations on the sortpion of cesium onto CuFC-EDA-GlyHMS and CuFC-AAHMS have been investigated. For CuFC-EDA-GlyHMS and CuFC-AAHMS composites, the cesium sorption was negligible in the presence of Na+ and Ca2+. It means that CuFC-EDA-GlyHMS and CuFC-AAHMS composites have cesium selectivity regardless of in the presence of the co-exitsitng cations.
Through thermodynamics studies, for CuFC-EDA-GlyHMS, cesium sorption occur by an endothermic process. All the sorption processes are spontaneous in nature according to the negative values of △G. For CuFC-AAHMS, cesium sorption occur by an endorhermic process and △H value for cesium indicates chemical sorption. All the sorption processes are spontaneous in nature according th the negative values of △G.
As a result, the two types of sorbents are combined in the synthesis method of the co-condensation. The co-condensation has stronger coherence of functional group than grafting. Thus, the co-condensation prevents copper ferrocyanide, which is combined with the sorbent, from leaching. CuFC-EDA-GlyHMS has mesoporous and a large surface area. Its equilibrium velocity is shorter than CuFC-AAHMS. To synthesize CuFC-AAHMS takes shorter time than to synthesize CuFC-EDA-GlyHMS. Also, CuFC-AAHMS has hight adsorption capacity to cesium.
These results make it possible to apply the developed materials for the selective removal of cesium in LIRW in practice.
목차
목 차················································································ⅰ표 목록············································································ⅳ그림 목록·········································································ⅵ1. 서론················································································12. 이론적 배경···································································32.1. 방사성 폐액의 발생 및 핵종의 특성····················32.2. 유기기능기가 결합된 실리카의 중금속 흡착······62.3. Ferrocyanide을 이용한 세슘 흡착······················122.4. 흡착속도 모델··························································172.5. 등온흡착 모델···························································212.6. 열역학적 연구···························································233. 실험재료 및 방법····························································253.1. 실험재료·····································································253.1.1. 시약·······································································253.1.2. 흡착제 합성··························································263.1.3. 물리화학적 특성분석··········································343.2. 실험방법······································································363.2.1. 흡착속도 실험 ······················································363.2.2. 등온흡착 실험 ······················································363.2.3. 비방사성 이온의 공존 영향································373.2.4. 열역학적 연구 ······················································384. 실험 결과 및 고찰····························································394.1. 물리화학적 특성분석·················································394.1.1. XRD·········································································394.1.2. TEM········································································484.1.3. SEM·········································································534.1.4. FT-IR·······································································564.1.5. 원소분석··································································624.1.6. 비표면적 및 기공도 분석······································704.2. 흡착속도 실험·······························································764.2.1. CuFC-EDA-GlyHMS·············································764.2.2. CuFC-AAHMS························································794.3. 등온흡착 실험································································824.3.1. CuFC-EDA-GlyHMS··············································824.3.2. CuFC-AAHMS·························································864.4. 비방사성 이온의 공존 영향··········································904.4.1. CuFC-EDA-GlyHMS··············································904.4.2. CuFC-AAHMS·························································964.5. 열역학적 연구································································1024.5.1. CuFC-EDA-GlyHMS·············································1024.5.2. CuFC-AAHMS························································1045. 결론·······················································································1066. 참고 문헌··············································································1097. 초록·······················································································114
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