本文關(guān)鍵詞： 溫室氣體 CO_2吸附劑 CO_2捕捉 TEPA　出處：《浙江師范大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

【摘要】：隨著工業(yè)化生產(chǎn)規(guī)模的迅猛擴大,以及化石燃料的大量燃燒,導(dǎo)致大氣中二氧化碳的含量不斷增加,這使得全球由溫室效應(yīng)引起的氣候變暖現(xiàn)象也在不斷加劇。因此,開發(fā)一種新型的二氧化碳分離和捕捉技術(shù),對于緩解氣候變暖是非常必要且迫切的。本論文分別采用P123為軟模板劑,1,2-二(三甲氧基硅基)乙烷(BTME);為硅源合成了介孔氧化硅納米管(E-SNTs)材料,E-SNTs經(jīng)過聚乙烯亞胺(PEI)修飾后制得吸附劑后用于CO2捕捉；表面活性劑F127作為軟模板劑,正硅酸四乙酯(TEOS)為硅源合成了有序介孔納米氧化硅OMS,通過負載有機胺TEPA制得OMS基吸附劑；以KIT-6為硬模板,乙二胺(EDA)為氮源、四氯化碳(CCl4)為碳源合成了炭基碳材料KIT-6-CN,并將三種材料用于CO2的捕獲。采用透射電鏡、N2吸脫附、熱重等儀器對其形貌及二氧化碳吸附性能進行了表征。1、氧化硅納米管基吸附劑的制備及其CO2吸附性能的研究制備一系列負載不同有機胺量的氧化硅納米管基吸附劑,并用于CO2的捕捉。結(jié)果表明,E-SNTs吸附劑的吸附性能隨著有機胺負載量的增加呈現(xiàn)了先增加后減小的趨勢,其中E-SNTs-50%(w)最大為3.32 mmol/g。這是因為該材料在負載有機胺的過程中,材料本身的孔徑會減小,導(dǎo)致氣體穿過時傳質(zhì)阻力變大。在通入C02氣體時帶入水汽,發(fā)現(xiàn)水汽不但沒有減弱吸附劑的吸附能力,反而起到了促進的作用,吸附量達到3.75 mmol/g。經(jīng)過多次吸脫附循環(huán)實驗證明了E-SNTs在負載有機胺后仍保持了較好的穩(wěn)定性和可再生性能。2、四乙烯五胺修飾不同孔徑OMS基吸附材料的制備及表征采用水熱法制備了不同孔徑的OMS材料,對其進行有機胺改性,并用于C02的捕捉。結(jié)果表明,OMS-7.6相比OMS-5.6因其具有較大的孔徑而在負載相同有機胺量時表現(xiàn)出更強的吸附性能。根據(jù)質(zhì)譜儀測試得到的穿透曲線可知,介孔孔徑越大,氣體在穿過吸附劑時傳質(zhì)阻力越小,則吸附劑的吸附能力越好。3、三維孔道KIT-6合成氮化碳材料的制備及表征以KIT-6材料為硬模板,制備氮摻雜的介孔碳材料KIT-6-CN用于CO2吸附性能研究測試。CO2吸脫附實驗結(jié)果顯示,KIT-6-CN比碳材料KIT-6-C有更好的CO2吸附性能,且在0℃時其吸附量(3.09 mmol/g)要大于25℃(2.11 mmol/g)時,這說明低溫有利于CO2的吸附。CO2循環(huán)實驗說明該材料具有良好的穩(wěn)定性。XPS結(jié)果證實,氮元素能促進碳材料對CO2吸附性能。
[Abstract]:With the rapid expansion of industrial production and the massive combustion of fossil fuels, the carbon dioxide content in the atmosphere is increasing. The global warming caused by Greenhouse Effect is also increasing. Therefore, a new CO2 separation and capture technology is being developed. It is very necessary and urgent to mitigate global warming. In this paper, we use P123 as a soft template, respectively, to use P123 (trimethoxysilyl) ethane (trimethoxysilyl) ethane butadiene (BTMEE) as a soft template. The mesoporous silica nanotubes (E-SNTs) were modified with polyvinyleneimide (PEI) to prepare an adsorbent for CO2 trapping. The surface active agent F127 was used as soft template and tetraethyl orthosilicate (TEOS) as silicon source to synthesize ordered mesoporous nano-silica OMSs. OMS based adsorbent was prepared by loading organic amine TEPA. Carbon based carbon material KIT-6-CN was synthesized by using KIT-6 as hard template, ethylenediamine as nitrogen source and carbon tetrachloride (CCL 4) as carbon source. Three kinds of materials were used to capture CO2. The morphology and carbon dioxide adsorption properties were characterized by transmission electron microscope (TEM) and N _ 2 adsorption and desorption, thermogravimetry and other instruments. Preparation of silica nanotube based adsorbents and their CO2 adsorption properties a series of silica nanotube based adsorbents loaded with different amounts of organic amines were prepared and used for CO2 trapping. The adsorption properties of E-SNTs adsorbent increased first and then decreased with the increase of the loading amount of organic amine. The maximum value of E-SNTs-50 is 3.32 mmol / g. This is because the pore size of the material decreases during the process of loading organic amine. It is found that water vapor not only does not weaken the adsorption ability of adsorbent, but also plays a promoting role. The adsorption capacity of E-SNTs was 3.75 mmol / g. After repeated desorption cycle experiments, it was proved that E-SNTs still maintained good stability and reproducibility of 2. 2 after loading organic amines. Preparation and characterization of OMS based adsorbents modified with tetraethylenepentylamine OMS materials with different pore sizes were prepared by hydrothermal method and modified with organic amines and used to capture C02. Compared with OMS-5.6, OMS-7.6 showed stronger adsorption performance when loaded with the same amount of organic amines because of its larger pore size. The larger the mesoporous pore size is, the smaller the mass transfer resistance of the gas is when it passes through the adsorbent, the better the adsorption capacity of the adsorbent is. 3. Preparation and characterization of carbon Nitride Materials synthesized by 3D pore KIT-6 with KIT-6 as hard template. Preparation of nitrogen-doped mesoporous carbon material KIT-6-CN for the study of the adsorption properties of CO2. KIT-6-CN has better CO2 adsorption performance than carbon material KIT-6-C. And at 0 鈩，

本文編號：1454979