本文關(guān)鍵詞：氧化鋁負(fù)載納米銅基脫硫劑的制備及脫硫效能研究　出處：《哈爾濱理工大學(xué)》2015年碩士論文　論文類(lèi)型：學(xué)位論文

  更多相關(guān)文章： 負(fù)載型納米脫硫劑 氧化銅 常溫脫硫 硫化氫 再生

【摘要】：為了提高納米脫硫劑活性組分利用率，提高脫硫活性，降低其使用成本，解決脫硫劑再生難等問(wèn)題，本研究擬開(kāi)發(fā)一種脫硫效果好，性能穩(wěn)定，可再生的負(fù)載型納米銅基脫硫劑，為工業(yè)化應(yīng)用提供技術(shù)參數(shù)。 論文采用等體積浸漬法和共沉淀法制備出氧化鋁負(fù)載型納米銅基脫硫劑，以H2S為目標(biāo)污染物，通過(guò)固定床反應(yīng)器對(duì)制備出的脫硫劑進(jìn)行脫硫活性評(píng)價(jià)，探討制備條件對(duì)脫硫活性的影響因素，確定最佳的制備工藝；利用多種測(cè)試技術(shù)對(duì)所制得負(fù)載型納米脫硫劑進(jìn)行表征，分析脫硫劑的結(jié)構(gòu)對(duì)脫硫效能的影響，并考察了助劑(Ce，F(xiàn)e，Co，Zn)對(duì)CuO/Al2O3脫硫活性和穩(wěn)定性的影響；探討再生溫度和再生氣氛等工藝對(duì)CuO/Al2O3再生性能的影響，并進(jìn)行多周期的硫化/再生循環(huán)實(shí)驗(yàn)。 結(jié)果表明共沉淀法制備脫硫劑脫硫效果明顯好于浸漬法，當(dāng)共沉淀劑為NaOH，焙燒溫度為400℃，，焙燒時(shí)間3h，活性組分最佳的負(fù)載比例70%時(shí)，H2S穿透時(shí)間為490min，硫容為140mg g-1，鈰摻雜到CuO/Al2O3中能使脫硫活性和穩(wěn)定性進(jìn)一步提高； 結(jié)構(gòu)分析顯示，共沉淀法制備的CuO/Al2O3中納米氧化銅的晶粒尺寸遠(yuǎn)小于浸漬法，且Al2O3抑制了氧化銅晶粒的生長(zhǎng)。采用XPS表征技術(shù)分析了CuO/Al2O3脫硫劑的硫化產(chǎn)物，結(jié)合硫化產(chǎn)物的TG曲線和XRD衍射圖，分析結(jié)果表明，存在著CuS和CuSO4兩種脫硫產(chǎn)物。 采用熱再生法在氧化或還原氛圍下對(duì)共沉淀法制備摻雜助劑的Ce-CuO/Al2O3，F(xiàn)e-CuO/Al2O3，Co-CuO/Al2O3，Zn-CuO/Al2O3樣品的再生性能進(jìn)行研究。研究表明，再生效果較好的脫硫劑是Ce-CuO/Al2O3和Zn-CuO/Al2O3。Ce-CuO/Al2O3納米脫硫劑在NH3氣氛下的再生效果要優(yōu)于氧氣氛，650℃時(shí)脫硫劑可進(jìn)行四次再生，累積脫硫劑穿透時(shí)間達(dá)803min，累積硫容達(dá)229.4mg·g-1；但Zn-CuO/Al2O3脫硫劑正相反，氧氣氛下的再生效果更好，600℃時(shí)四次再生后的累積H2S穿透時(shí)間達(dá)755min，累積硫容達(dá)215.7mg g-1。
[Abstract]:In order to improve the utilization rate of desulfurizer activated nano group, improve the desulfurization activity, reduce its cost, solve the problem of desulfurizer regeneration difficult, this study intends to develop a good desulfurization effect, stable performance, supported nano copper based sorbents renewable, provide technical parameters for the industrial application.
The paper by impregnation method and were prepared by nano copper based sorbents supported on alumina, taking H2S as a target pollutant, the desulfurization activity evaluation of desulfurization agent for the preparation by fixed bed reactor, to explore the influence factors of preparation conditions on the desulfurization activity, determine the best preparation process of; prepared were characterized using a variety of desulfurization agent supported nano testing technology, structure analysis of desulfurization agent on desulfurization efficiency, and the effects of additives (Ce, Fe, Co, Zn) of CuO/Al2O3 desulfurization activity and stability; to explore the effects of regeneration temperature and regeneration atmosphere regeneration process on the performance of CuO/Al2O3, sulfide / and multi cycle recycling experiments.
The results show that the coprecipitation desulfurization effect is obviously better than the impregnation method, the co precipitation agent NaOH, calcination temperature of 400 DEG 3h, roasting time, active component load ratio of 70% when the optimal H2S penetration time is 490min, the sulfur content of 140mg g-1, CE doped into CuO/Al2O3 can make the desulfurization activity and further improve the stability;
The structure analysis shows that the grain size of nano copper oxide prepared by CuO/Al2O3 is much smaller than the impregnation coprecipitation, and the inhibition of Al2O3 copper oxide grain growth. Analysis of sulfurized CuO/Al2O3 desulfurizer characterized by XPS technology, combined with the curing product TG curve and XRD diffraction analysis results show that the existence of CuS and CuSO4 two kinds of desulfurization products.
The thermal regeneration method in oxidizing or reducing atmosphere on the preparation of doped additives by coprecipitation method Ce-CuO/Al2O3, Fe-CuO/Al2O3, Co-CuO/Al2O3, Zn-CuO/Al2O3 of regeneration performance of samples. The results show that better regeneration desulfurization agent is Ce-CuO/Al2O3 and Zn-CuO/Al2O3.Ce-CuO/ regeneration effect of Al2O3 nano desulfurizing agent in NH3 atmosphere is better than that of oxygen atmosphere at 650 DEG. The desulfurization agent can be four times the cumulative desulfurizer regeneration, the breakthrough time was 803min, the cumulative sulfur capacity 229.4mg g-1; but Zn-CuO/Al2O3 desulfurizing agent on the contrary, better regeneration effect in oxygen atmosphere at 600 DEG C, the cumulative H2S after four times regeneration penetration time was 755min, the cumulative sulfur capacity of 215.7mg g-1.

【學(xué)位授予單位】：哈爾濱理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類(lèi)號(hào)】：X701.3

【參考文獻(xiàn)】

相關(guān)期刊論文 前10條

1 張春燕;劉宇紅;趙文輝;;生物脫硫技術(shù)在煉廠氣中的應(yīng)用[J];化學(xué)工業(yè);2008年03期

2 趙瑞壯;上官炬;婁艷茹;宋瑾;;高溫煤氣脫硫劑再生行為氣氛效應(yīng)的研究進(jìn)展[J];化工進(jìn)展;2010年04期

3 周繼紅,華玉芝,史長(zhǎng)林,連延軍;負(fù)載型活性炭脫硫(H_2S)的試驗(yàn)研究[J];河北建筑科技學(xué)院學(xué)報(bào);2003年01期

4 張密林,張紅霞,陳野;(鋅、銅、錳)復(fù)合脫硫劑的制備及性能研究[J];化學(xué)工業(yè)與工程技術(shù);2004年06期

5 張長(zhǎng)拴,趙峰,張繼軍,王向宇,鮑改玲,白玉白,李鐵津;納米尺寸氧化鋁的紅外光譜研究[J];化學(xué)學(xué)報(bào);1999年03期

6 譚小耀,吳迪鏞,袁權(quán);浸漬活性炭脫除低濃度H_2S的研究[J];化學(xué)工程;1996年06期

7 王芳芳;趙海;張德祥;高晉生;;鐵錳系脫硫劑對(duì)煤氣中羰基硫的脫硫機(jī)理初探[J];煤炭學(xué)報(bào);2008年02期

8 高春珍;梁美生;李春虎;樊惠玲;;氧化鈰高溫煤氣脫硫劑制備條件對(duì)脫硫效率的影響[J];煤炭學(xué)報(bào);2011年02期

9 宋華;羅威;許林祥;張嬌靜;;Al_2O_3/Fe_2O_3吸附劑脫除硫化氫的性能[J];化工進(jìn)展;2013年04期

10 孫振麗;楊新芳;田文棟;趙麗鳳;肖云漢;;共沉淀法制備鐵鋅基中高溫煤氣脫硫劑[J];環(huán)境工程學(xué)報(bào);2014年02期

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