活性炭基催化劑制備及液化氣中脫硫機(jī)理研究
發(fā)布時(shí)間:2018-02-16 20:36
本文關(guān)鍵詞: 活性炭 改性 羰基硫 水解催化劑 出處:《青島科技大學(xué)》2017年碩士論文 論文類型:學(xué)位論文
【摘要】:隨著人類對石油等資源需求量的不斷加大,原油劣質(zhì)化的日益嚴(yán)重,各國更加嚴(yán)格的環(huán)保要求,人們越來越受到重視生產(chǎn)更加清潔的石油化工產(chǎn)品。而實(shí)現(xiàn)生產(chǎn)更加清潔能源產(chǎn)品的目標(biāo),重要手段之一就是研發(fā)更加高效的脫硫催化劑。本文主要從催化劑載體改性和催化劑制備等方面進(jìn)行了較為系統(tǒng)的研究。本文對載體活性炭改性進(jìn)行了研究,主要考察了活性炭預(yù)處理、活性炭堿改性對載體活性炭表面性質(zhì)及脫硫活性的影響。經(jīng)去離子水和鹽酸的預(yù)處理使活性炭的比表面積和孔容增加;對活性炭進(jìn)行堿改性,在一定程度上降低了活性炭的比表面積和總孔容,但脫硫效果卻明顯提高,這是由于堿改性增加了活性炭表面的堿性基團(tuán)的含量,促使羰基硫水解生成硫化氫,水解后產(chǎn)物硫化氫經(jīng)氧化,最終在活性炭表面生成單質(zhì)硫或硫酸鹽。本文進(jìn)行了Cu/AC水解催化劑和Cu-Fe/AC水解催化劑的制備及脫硫性能的研究,并采用BET、XRD和SEM等表征方法對催化劑樣品進(jìn)行了表征,評價(jià)了催化劑的脫硫活性。實(shí)驗(yàn)對Cu/AC水解催化劑主要從制備方法、活性組分添加量、焙燒溫度和堿負(fù)載量四個(gè)方面展開研究,而對于Cu-Fe/AC水解催化劑則主要從雙組分添加順序、摩爾比和催化劑的工藝條件三個(gè)方面展開研究。研究結(jié)果表明,采用浸漬法制備的Cu/AC水解催化劑,活性組分銅的最佳負(fù)載量為7wt%,最佳焙燒溫度為350℃,堿最佳添加量為11wt%,此時(shí)水解催化劑的硫容為29 mgS/g。對于雙組分負(fù)載的Cu-Fe/AC水解催化劑,先浸漬鐵后浸漬銅制備出的水解催化劑脫硫活性最高,雙組份最佳摩爾比為5:1;催化劑最佳工藝條件為:反應(yīng)溫度為70℃,濕度為32%,最佳空速為1200h~(-1)。
[Abstract]:With the increasing demand for oil and other resources, the deterioration of crude oil is becoming more and more serious, and the environmental protection requirements of various countries are more stringent. More and more attention is being paid to producing cleaner petrochemical products, and to achieving the goal of producing cleaner energy products. One of the important means is to develop more efficient desulfurization catalyst. This paper mainly studies the modification of catalyst carrier and preparation of catalyst. The effects of activated carbon pretreatment and alkali modification on the surface properties and desulfurization activity of activated carbon were investigated. The specific surface area and pore volume of activated carbon were increased by pretreatment with deionized water and hydrochloric acid. To some extent, the specific surface area and total pore volume of activated carbon were reduced, but the desulfurization effect was improved obviously, which was due to the alkali modification increased the content of basic group on the surface of activated carbon and promoted the hydrolysis of carbonyl sulfur to form hydrogen sulfide. After the hydrolysis, hydrogen sulfide was oxidized to form elemental sulfur or sulfate on the surface of activated carbon. The preparation and desulfurization performance of Cu/AC hydrolysis catalyst and Cu-Fe/AC hydrolysate catalyst were studied in this paper. The catalyst sample was characterized by BET-XRD and SEM, and the desulfurization activity of the catalyst was evaluated. The calcination temperature and alkali loading were studied in four aspects, while the Cu-Fe/AC hydrolysis catalyst was mainly studied from three aspects: the order of adding two components, the molar ratio and the process conditions of the catalyst. The Cu/AC hydrolysis catalyst prepared by impregnation method, the best loading amount of active component copper is 7 wts. the optimum calcination temperature is 350 鈩,
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