【摘要】：隨著環(huán)保要求的提高,涉汞催化劑的替代已成為電石法聚氯乙烯產業(yè)發(fā)展的瓶頸。炭基非金屬無汞催化劑具有成本低廉,耐腐蝕性及耐熱性能好等特點,是目前無汞觸媒研發(fā)中的一個重要方向。本論文對商品活性炭的表面改性及中孔淀粉炭的制備方法進行了研究,關聯(lián)了炭材料的表面化學基團、灰分、氮摻雜等和乙炔氫氯化催化性能之間的關系,得到以下結論:1.商業(yè)活性炭的表面羧基等酸性含氧基團含量越高,乙炔氫氯化活性及穩(wěn)定性越差;活性炭的灰分含量越低,催化劑活性越好;在比表面積、灰分、孔隙結構都接近的情況下,不同來源的活性炭乙炔氫氯化反應活性順序如下:煤質炭木質炭椰殼炭,其活性可能和活性炭的石墨化程度有關。2.商品活性炭通過尿素改性可引入含氮基團,氮含量隨焙燒溫度的降低而提高,改性后的活性炭乙炔氫氯化活性隨氮含量的提高而線性增加。3.以小麥淀粉為碳源,采用固相研磨的硬模板法,成功制備了成型的中孔淀粉炭,和活性炭及蔗糖為碳源制備的中孔炭相比,中孔淀粉炭具有更好的乙炔氫氯化催化性能。在固相碾磨的過程中可加入三聚氰胺調節(jié)氮含量。當炭材料中的氮含量低于4%時,氮摻雜中孔淀粉炭的乙炔氫氯化活性隨氮含量增加而增加;當氮含量高于4%時,其乙炔轉化率基本不變。
[Abstract]:With the improvement of environmental protection requirements, the substitution of mercury-related catalysts has become the bottleneck of the development of calcium carbide polyvinyl chloride industry. Carbon-based non-metallic mercury-free catalysts have the advantages of low cost, good corrosion resistance and heat resistance, which is an important direction in the research and development of mercury-free catalysts. In this paper, the surface modification of commercial activated carbon and the preparation of mesoporous starch carbon were studied. The relationship between the surface chemical groups, ash, nitrogen doping and catalytic properties of acetylene hydrochlorination was studied. The higher the content of acidic oxygen groups such as carboxyl group on the surface of commercial activated carbon, the worse the activity and stability of hydrogen chlorination of acetylene; the lower the ash content of activated carbon, the better the activity of catalyst; when the specific surface area, ash and pore structure are close to each other, The order of activity of acetylene hydrochlorination of activated carbon from different sources is as follows: the activity of charcoal wood coconut shell charcoal may be related to the graphitization degree of activated carbon. Commercial activated carbon can introduce nitrogen-containing groups through urea modification, the nitrogen content increases with the decrease of calcination temperature, and the hydrogen-chlorination activity of modified activated carbon increases linearly with the increase of nitrogen content. Mesoporous starch carbon was successfully prepared by solid phase grinding with wheat starch as carbon source. Compared with activated carbon and sucrose as carbon source, mesoporous starch carbon has better catalytic performance for hydrogen acetylene chlorination. Melamine can be added to adjust nitrogen content in the process of solid-phase milling. When the nitrogen content in carbon is lower than 4, the activity of acetylene hydrochlorination of N-doped mesoporous starch carbon increases with the increase of nitrogen content, but when nitrogen content is higher than 4, the conversion rate of acetylene is almost unchanged.
【學位授予單位】：浙江工業(yè)大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O643.36

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