光響應(yīng)載體負(fù)載的鐵基和鈷基催化劑的合成及光熱催化費(fèi)托合成反應(yīng)性能
本文選題:費(fèi)托合成 切入點(diǎn):光熱催化 出處:《內(nèi)蒙古大學(xué)》2017年碩士論文
【摘要】:費(fèi)托合成(FTS)是以合成氣(CO+H_2)為原料在催化劑和適當(dāng)?shù)臈l件下合成以長(zhǎng)鏈烷烴為主的清潔液體燃料過(guò)程,是應(yīng)對(duì)當(dāng)前日益凸顯的能源危機(jī)的最有效途徑之一。而光熱費(fèi)托合成是在傳統(tǒng)熱費(fèi)托的基礎(chǔ)上引入光源,研究光熱驅(qū)動(dòng)的費(fèi)托合成反應(yīng)。為打破傳統(tǒng)ASF分布規(guī)律提供新思路,對(duì)于能源資源的清潔、高效利用具有深刻意義。論文選取半導(dǎo)體SiC和CoAl_2O_4作為光響應(yīng)載體,Fe和Co作為熱敏感活性組分制備了一系列雙功能催化劑并在不同條件下進(jìn)行了催化活性評(píng)價(jià)。主要得到了如下研究結(jié)果:(1)以在可見(jiàn)光區(qū)有吸收的非金屬半導(dǎo)體SiC為載體制備了 15%Co/SiC催化劑,對(duì)其進(jìn)行了熱及光熱條件下的催化活性測(cè)試,發(fā)現(xiàn)引入光源后CO的轉(zhuǎn)化率升高,CH_4選擇性降低,C5+選擇性升高,C_2-C_4產(chǎn)物中烷烴比例上升,烯烴比例下降。說(shuō)明光源的引入有利于CO轉(zhuǎn)化和碳鏈增長(zhǎng)。這與以非光活性Si02為載體光熱催化的規(guī)律不同。(2)以CoAl_2O_4和CoAl_2O_4-A1_2O_3為載體,負(fù)載15%Co作為催化劑,分別進(jìn)行了熱及光熱費(fèi)托活性評(píng)價(jià),結(jié)果發(fā)現(xiàn)引入光源后兩種催化劑的活性變化規(guī)律相同。與熱催化相比,CO轉(zhuǎn)化率大幅提高,CH_4的選擇性降低,C__(5+)選擇性升高,C_2-C_4產(chǎn)物中烷烯比升高,說(shuō)明引入光源有利于CO的轉(zhuǎn)化和Co的還原。但是在相同反應(yīng)條件下,15%Co/CoAl_2O_4-Al_2O_3催化劑的活性比15%Co/CoAl_2O_4高,因?yàn)镃oAl_2O_4-Al_2O_3中存在界面效應(yīng)。同時(shí)對(duì)15%Co/CoAl_2O_4-Al_2O_3催化劑在引入不同光源的條件下進(jìn)行了活性測(cè)試,發(fā)現(xiàn)引入可見(jiàn)光時(shí)催化活性最高。(3)以Fe為熱活性組分制備了 15%Fe/SiC催化劑,分別進(jìn)行了熱催化及光熱催化活性測(cè)試,發(fā)現(xiàn)引入光源后CO的轉(zhuǎn)化率提高,CO_2的選擇性降低,C_(5+)選擇性升高,C_2-C_4產(chǎn)物中烷烯比升高。在反應(yīng)過(guò)程中生成的碳納米纖維促進(jìn)了反應(yīng)的進(jìn)行。
[Abstract]:FTS is a process of synthesizing clean liquid fuel with long chain alkanes as the main fuel under the condition of catalyst and suitable conditions. It is one of the most effective ways to deal with the energy crisis which is becoming more and more prominent at present.The photothermal Fischer synthesis is based on the traditional heat Fischer to introduce the light source to study the photothermal driven Fischer synthesis reaction.It is of great significance for clean and efficient utilization of energy resources to break the traditional ASF distribution rule.In this paper, a series of bifunctional catalysts were prepared using semiconductor SiC and CoAl_2O_4 as photo-response carriers, Fe and Co as heat-sensitive active components, and the catalytic activity was evaluated under different conditions.The main results are as follows: (1) the 15%Co/SiC catalyst was prepared on the support of non-metallic semiconductor SiC, which was absorbed in the visible light region, and its catalytic activity was tested under thermal and photothermal conditions.It is found that the conversion rate of CO increases with the introduction of light source; the selectivity of CHS _ 4 decreases; the selectivity of C _ 5 increases; the proportion of alkanes in C _ 2-C _ 4 products increases and the ratio of olefins decreases.The results show that the introduction of light source is beneficial to CO conversion and carbon chain growth.This is different from that of photothermal catalysis using non-photoactive Si02 as the carrier. The photothermal and photothermal Fischer-Tropsch activity were evaluated using CoAl_2O_4 and CoAl_2O_4-A1_2O_3 as supports and supported 15%Co as catalyst, respectively.The results showed that the activity of the two catalysts was the same when the light source was introduced.Compared with thermal catalysis, the conversion rate of CO is greatly increased. The selectivity of Ch _ 4 is reduced. (C _ S _ S _ (5)) the ratio of alkane to ene in C _ 2-C _ 4 products is increased, indicating that the introduction of light source is beneficial to the conversion of CO and the reduction of Co.But under the same reaction conditions, the activity of Co/ CoAl _ 2O _ 3 catalyst is higher than that of 15%Co/CoAl_2O_4 because of the interfacial effect in CoAl_2O_4-Al_2O_3.At the same time, the activity of 15%Co/CoAl_2O_4-Al_2O_3 catalyst was tested under the condition of introducing different light sources. It was found that the catalytic activity of 15%Co/CoAl_2O_4-Al_2O_3 catalyst was the highest when the visible light was introduced. (3) the 15% sic catalyst was prepared with Fe as the thermal active component.Thermal catalysis and photothermal catalytic activity tests were carried out respectively. It was found that the conversion rate of CO increased with the introduction of light source. The selectivity of CO _ 2 was decreased. (C _ S _ 5) the ratio of alkene to alkene in the products of C _ 2-C _ 4 was higher than that of C _ (2) C _ (4).The reaction was facilitated by carbon nanofibers generated during the reaction.
【學(xué)位授予單位】:內(nèi)蒙古大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類(lèi)號(hào)】:O643.36;TQ529.2
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