活性炭基催化剂制备及液化气中脱硫机理研究

发布时间：2018-02-16 20:36

  本文关键词： 活性炭 改性 羰基硫 水解催化剂　出处：《青岛科技大学》2017年硕士论文　论文类型：学位论文

【摘要】：随着人类对石油等资源需求量的不断加大,原油劣质化的日益严重,各国更加严格的环保要求,人们越来越受到重视生产更加清洁的石油化工产品。而实现生产更加清洁能源产品的目标,重要手段之一就是研发更加高效的脱硫催化剂。本文主要从催化剂载体改性和催化剂制备等方面进行了较为系统的研究。本文对载体活性炭改性进行了研究,主要考察了活性炭预处理、活性炭碱改性对载体活性炭表面性质及脱硫活性的影响。经去离子水和盐酸的预处理使活性炭的比表面积和孔容增加;对活性炭进行碱改性,在一定程度上降低了活性炭的比表面积和总孔容,但脱硫效果却明显提高,这是由于碱改性增加了活性炭表面的碱性基团的含量,促使羰基硫水解生成硫化氢,水解后产物硫化氢经氧化,最终在活性炭表面生成单质硫或硫酸盐。本文进行了Cu/AC水解催化剂和Cu-Fe/AC水解催化剂的制备及脱硫性能的研究,并采用BET、XRD和SEM等表征方法对催化剂样品进行了表征,评价了催化剂的脱硫活性。实验对Cu/AC水解催化剂主要从制备方法、活性组分添加量、焙烧温度和碱负载量四个方面展开研究,而对于Cu-Fe/AC水解催化剂则主要从双组分添加顺序、摩尔比和催化剂的工艺条件三个方面展开研究。研究结果表明,采用浸渍法制备的Cu/AC水解催化剂,活性组分铜的最佳负载量为7wt%,最佳焙烧温度为350℃,碱最佳添加量为11wt%,此时水解催化剂的硫容为29 mgS/g。对于双组分负载的Cu-Fe/AC水解催化剂,先浸渍铁后浸渍铜制备出的水解催化剂脱硫活性最高,双组份最佳摩尔比为5:1;催化剂最佳工艺条件为:反应温度为70℃,湿度为32%,最佳空速为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，

本文编号：1516383