本文關(guān)鍵詞：載體對Pd-Fe雙金屬吸附劑中溫煤氣脫汞活性及再生性能影響的研究　出處：《太原理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 煤氣 雙金屬吸附劑 脫汞 再生性能

【摘要】：煤氣化是現(xiàn)代煤化工的基礎(chǔ),是應(yīng)用最廣泛的潔凈煤技術(shù)之一,具有效率高,應(yīng)用廣泛等優(yōu)點(diǎn)。而煤氣化過程中的煤氣是還原性氣氛,比煤燃燒產(chǎn)生的氣量小,導(dǎo)致其釋放的單質(zhì)汞遠(yuǎn)高于燃煤煙氣。單質(zhì)汞具有神經(jīng)毒性和生物累積性,對人類健康和生態(tài)環(huán)境具有嚴(yán)重危害;單質(zhì)汞又具有極高的揮發(fā)性、微溶于水和化學(xué)性質(zhì)穩(wěn)定等特點(diǎn),與其他形式的汞相比,其最難除去。因此,研發(fā)脫汞性能優(yōu)異的吸附劑顯得尤其重要,同時(shí)為了使汞脫除劑在工業(yè)中能夠得到應(yīng)用,大大的降低商業(yè)化運(yùn)營成本,對汞吸附飽和后的吸附劑進(jìn)行再生處理,研究具有良好再生性能的脫汞劑具有重要的現(xiàn)實(shí)意義。本課題組前期考察了用等體積浸漬法、共沉淀法和溶劑熱法制備Pd-Fe雙金屬吸附劑在中溫模擬煤氣中的脫汞性能,實(shí)驗(yàn)結(jié)果證明Pd-Fe雙金屬吸附劑優(yōu)異的脫汞活性,同時(shí)進(jìn)一步研究了吸附劑制備條件和脫汞實(shí)驗(yàn)條件對吸附劑脫汞活性的影響。本論文在此基礎(chǔ)上選擇以Beta分子篩、活性炭和γ-Al2O3作為載體,以貴金屬Pd和Fe2O3作為脫汞活性組分,用等體積浸漬法和共沉淀法制備Pd-Fe雙金屬負(fù)載型吸附劑,重點(diǎn)考察了三種載體對吸附劑脫汞活性和再生性能的影響以及氣氛對吸附劑脫汞活性的影響,并結(jié)合XRD、CO脈沖吸附、FTIR、XPS、BET和Hg0-TPD等表征結(jié)果,探討載體對吸附劑的影響。得到如下主要結(jié)論:(1)載體對等體積浸漬法制備Pd-Fe雙金屬吸附劑的脫汞活性具有明顯的影響。Pd-Fe/AC吸附劑的脫汞活性最好,脫汞效率在480 min后可以保持在95%左右。其次是Pd-Fe/Beta吸附劑,脫汞效率在480 min后可以保持在90%左右。Pd-Fe/Al2O3吸附劑的脫汞活性最差,脫汞效率在480min內(nèi)從98%減小到75%。分析結(jié)果表明,Pd-Fe/AC吸附劑上活性組分Pd0的表面含量最高,Pd-Fe/Beta次之,Pd-Fe/Al2O3最小,同時(shí)Pd在Pd-Fe/AC吸附劑的分散度最好,Pd-Fe/Al2O3最差,從而導(dǎo)致Pd-Fe/AC的脫汞活性最好,Pd-Fe/Al2O3的脫汞活性最差。(2)載體對等體積浸漬法制備Pd-Fe雙金屬吸附劑再生性能影響較大。其中Pd-Fe/AC的再生性能最好,第一次脫汞效率在400 min內(nèi)仍保持在95%以上,經(jīng)過4次再生后,脫汞效率逐漸降低但仍保持在80%左右。其次是Pd-Fe/Beta吸附劑,初次脫汞效率在400 min內(nèi)保持在90%左右,經(jīng)過4次再生后,其脫汞效率逐漸降低但仍保持在75%左右。而Pd-Fe/Al2O3吸附劑再生性能最差,經(jīng)4次再生后,其脫汞效率僅為25%。其原因是在再生實(shí)驗(yàn)中,Pd-Fe/Al2O3吸附劑上生成了較多的Pd S,導(dǎo)致活性組分Pd0含量降低,而Pd S在脫附中不能分解產(chǎn)生Pd0,從而Pd-Fe/Al2O3吸附劑的脫汞效率下降快,再生性能較差。(3)共沉淀法制備雙金屬吸附劑載體對其再生性能的影響較小,且其規(guī)律一致。Pd-Fe/AC吸附劑初次脫汞活性在400 min內(nèi)保持在95%以上,經(jīng)過4次再生后,其脫汞效率逐漸降低但仍保持在80%左右。Pd-Fe/Beta和Pd-Fe/Al2O3吸附劑的初次脫汞活性在400 min內(nèi)保持在90%以上,經(jīng)過4次再生后,其脫汞效率逐漸降低但仍保持在75%左右。(4)煤氣中H_2S,H_2和CO對共沉淀法制備Pd-Fe/AC、Pd-Fe/Beta和Pd-Fe/Al2O3吸附劑脫汞活性的影響規(guī)律基本一致。H_2S氣氛對吸附劑脫汞活性有明顯抑制作用,這可能是加入的H_2S與Fe2O3反應(yīng)生成S0,S0與Pd0反應(yīng)生成Pd S使活性組分Pd0中毒,從而致使吸附劑的脫汞效率下降。H_2和CO氣氛對吸附劑脫汞活性有明顯促進(jìn)作用,這可能是H_2和CO的加入會(huì)緩慢還原出活性組分Pd0,從而提高吸附劑的脫汞效率。
[Abstract]:Coal gasification is the foundation of modern coal chemical industry, clean coal technology is one of the most widely used, has the advantages of high efficiency, wide application. But in the coal gasification gas is reducing atmosphere than coal combustion gas is small, resulting in the release of mercury is much higher than that of coal-fired flue gas mercury neurotoxicity has. And bioaccumulation, with serious harm to human health and ecological environment; mercury has a high volatile, slightly soluble in water and the characteristics of chemical stability, compared with other forms of mercury, the most difficult to remove. Therefore, developing excellent adsorbent for mercury removal is particularly important, at the same time in order to make mercury removal agent can be applied in the industry, greatly reduce the cost of commercial operation, carry out regeneration adsorption of mercury after adsorption agent, has important practical significance to study the mercury removal agent has good regeneration performance. Ourprevious study by impregnation method, method and solvothermal synthesis of Pd-Fe double metal adsorbent in temperature simulation of mercury removal characteristic in gas co precipitation. The experimental results show that the Pd-Fe double metal adsorbent for mercury removal activity excellent, and further research the preparation conditions and the mercury removal effect of experimental conditions for mercury removal on the activity of adsorption agent. This paper chooses Beta molecular sieve, activated carbon and gamma -Al2O3 as the carrier, with the noble metal Pd and Fe2O3 as the active component for mercury removal, impregnation method and co precipitation method to prepare Pd-Fe double metal supported adsorbent, emphasis on the three effect of adsorbent carrier on mercury removal activity and regeneration performance and the atmosphere on the adsorbent for mercury removal activity, combined with XRD, CO FTIR, XPS, pulse adsorption, BET and Hg0-TPD characterization results, to explore the influence of carrier on the adsorbent. The main results are summarized as follows. Theory: (1) preparation has obvious effect of mercury removal activity of.Pd-Fe/AC adsorbent for mercury removal activity best Pd-Fe bimetallic sorbent carrier equal volume impregnation method, mercury removal efficiency can be maintained at around 95% in 480 after min. The second is Pd-Fe/Beta adsorbent, mercury removal efficiency at 480 min can be maintained at around 90%.Pd-Fe/Al2O3 adsorbent for mercury removal activity is the worst, the mercury removal efficiency of 480min decreased from 98% to 75%. analysis results show that the surface content of Pd0 Pd-Fe/AC group activity adsorbent was highest, followed by Pd-Fe/Beta, Pd-Fe/Al2O3 and Pd in the Pd-Fe/AC minimum, the best dispersion of absorbing agent, Pd-Fe/Al2O3 is the worst, which lead to Pd-Fe/AC the mercury removal activity is best, Pd-Fe/Al2O3 activity of mercury removal is the worst. (2) preparation of Pd-Fe double metal adsorbent regeneration has great influence on equal volume impregnation method. The carrier regeneration performance of Pd-Fe/AC is the best, the first time the mercury removal efficiency in 4 In 00 min remained at more than 95%, after the 4 regeneration, mercury removal efficiency gradually decreased but remained at around 80%. The second is Pd-Fe/Beta adsorbent, initial mercury removal efficiency in 400 min remained at around 90%, after the 4 regeneration, the mercury removal efficiency gradually decreased but remained at around 75%. While the Pd-Fe/Al2O3 adsorbent regeneration performance is the worst, after 4 times of regeneration, the mercury removal efficiency was only 25%., its reason is in the regeneration experiment, Pd-Fe/Al2O3 adsorbent to generate more Pd S, leading to the active components of Pd0 and Pd decreased, S in high school and can not be decomposed into Pd0, and the removal of mercury Pd-Fe/Al2O3 adsorption efficiency decreased quickly, the regeneration performance is poor. (3) preparation of double metal adsorbent has little effect on the performance of carrier regeneration co precipitation method, and the regularity of.Pd-Fe/AC adsorbent initial mercury removal activity within 400 min remained above 95% after 4 times of regeneration after its removal The efficiency of mercury decreased gradually but still maintain the first.Pd-Fe/Beta at about 80% Pd-Fe/Al2O3 and adsorbent for mercury removal activity within 400 min remained above 90% after 4 times of regeneration, the mercury removal efficiency gradually decreased but remained at around 75%. (4) the gas in H_2S, H_2 and CO on Pd-Fe/AC by co precipitation method for Pd-Fe/Beta and Pd-Fe/Al2O3 adsorbents for mercury removal activity of similar.H_2S atmosphere has obvious inhibitory effects on adsorption of mercury removal activity, which may be H_2S and Fe2O3 reaction of S0 with the reaction of S0 and Pd0 Pd S to generate the active components of Pd0 poisoning, resulting in adsorbents for mercury removal efficiency decreased by.H_2 and CO atmosphere on the adsorbent for mercury removal activity has obvious effect, which may be H_2 and CO will add the slow reduction of the active components of Pd0, so as to improve the efficiency of mercury removal adsorbent.

【學(xué)位授予單位】：太原理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TQ546.5

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