论文总字数：18151字

摘 要

本文以MIL-101(Cr)-NH₂为吸附剂，93#汽油蒸汽（简称油气）为吸附质，考察了MIL-101(Cr)-NH₂对油气的动态吸附及抽再生性能，采用BET对抽真空前后的MIL-101(Cr)-NH₂进行表征。结果表明：

1. MIL-101(Cr)-NH₂对油气适宜的吸附工艺条件为：进料浓度20-50g/m³，吸附温度30°C，吸附压力0.1MPa，进料体积空速77.3h^-1，以油气浓度25mg/m³为穿透点，MIL-101(Cr)-NH₂对油气的穿透吸附量为0.74mg/g_ads。
2. MIL-101(Cr)-NH₂对油气适宜的真空再生工艺条件为：再生压力10mbar，再生温度30°C，再生时间40min时MIL-101(Cr)-NH₂对油气的再生效率为61.7%；经过七次真空再生循环后，MIL-101(Cr)-NH₂的再生效率稳定在42%左右。
3. 对MIL-101(Cr)-NH₂和抽真空再生一次后的MIL-101(Cr)-NH₂-R的BET表征结果显示：与MIL-101(Cr)-NH₂相比，MIL-101(Cr)-NH₂-R中微孔和介孔孔体积恢复率超过95%，其介孔与微孔的孔道均匀性增加，互相连通的多级孔增多，有利于再生过程中吸附质的脱附。

关键词：MIL-101(Cr)-NH₂ 93#汽油蒸汽 吸附 再生

Research on dynamic adsorption and regeneration performance of MIL-101(Cr)-NH₂ for 93 # gasoline vapor

ABSTRACT

In this paper, amino-functionalized MIL-101(Cr)-NH₂ was used as adsorbent, 93 # gasoline vapor (named as gasoline vapor) was used as adsorbate, dynamic adsorption performance and regeneration performance of MIL-101(Cr)-NH₂ for gasoline vapor were investigated. MIL-101(Cr)-NH₂ before and after vacuum were characterized by BET. The results were showed as follows.

1. The suitable dynamic adsorption conditions of MIL-101(Cr)-NH₂ for gasoline vapor were feed concentration 20-50 g/m³, adsorption temperature 30°C, adsorption pressure 0.1 MPa, feed volume space velocity 77.3 h^-1, When the breakthrough concentration of gasoline vapor was 25 mg/m³, the breakthrough adsorption capacity of MIL-101(Cr)-NH₂ for gasoline vapor was 0.74 mg/g_ads.
2. The suitable vacuum regeneration conditions of MIL-101(Cr)-NH₂ for gasoline vapor were regeneration pressure 10 mbar, regeneration temperature 30°C, regeneration time 40 min, the regeneration efficiency of MIL-101(Cr)-NH₂ was 61.7%. After seven vacuum regeneration cycles, the regeneration efficiency of MIL-101(Cr)-NH₂ still kept 42%.
3. BET results of MIL-101(Cr)-NH₂ and MIL-101(Cr)-NH₂-R (regenerated by vacuum one time) showed that compared to MIL-101(Cr), regeneration efficiency of micropores volume and mesopores volume was more than 95% in MIL-101(Cr)-NH₂-R. The increases of hierarchical pores made the pore uniformity, which were beneficial to desorption of the adsorbates in the regeneration process of MIL-101(Cr)-NH₂.

Key Words: MIL-101(Cr)-NH₂; 93# gasoline vapor; Adsorption; Regeneration

目 录

摘要 I

ABSTRACT II

第一章 概述 1

1.1 研究背景与意义 1

1.2 用于油气回收吸附剂的研究进展 1

1.2.1 活性炭 1

1.2.2 疏水硅胶 1

1.2.3 分子筛 2

1.3 MOFs材料用于VOCs吸附净化研究进展 2

1.3.1 MOFs材料 2

1.3.2 MOFs材料改性 3

1.3.3 MOFs材料再生 3

1.4 本文主要研究内容 4

第二章 实验 5

2.1 主要原料及仪器 5

2.1.1 原料及试剂 5

2.1.2 主要仪器及设备 6

2.2 MIL-101(Cr)-NH₂合成 6

2.3油气动态吸附及再生实验 6

2.4 吸附剂的比表面积及孔体积表征 7

第三章 结果与讨论 9

3.1 MIL-101(Cr)-NH₂对油气动态吸附性能 9

3.1.1 空速 9

3.1.2 吸附温度 10

3.2 MIL-101(Cr)-NH₂抽真空再生工艺 11

3.2.1 抽真空温度 11

3.2.2 抽真空压力 11

3.2.3 抽真空时间 12

3.2.4 MIL-101(Cr)-NH₂抽真空再生稳定性 13

3.3 MIL-101(Cr)-NH₂和MIL-101(Cr)-NH₂-R的孔结构表征 14

第四章 结论与展望 16

4.1 结论 16

4.2 展望 16

参考文献 17

致谢 19

第一章 概述

1.1 研究背景与意义

汽油由多种有机化合物构成，其主要成分是C₄-C₁₂脂肪烃和环烃，以其为代表的轻质油品在制造、存储、输送、销售和使用过程中也会因挥发问题而产生汽油蒸汽类VOCs。这些汽油蒸汽挥发到空气中不仅造成环境污染、危害人体健康^[1]，更容易形成火灾隐患，且造成巨大的资源浪费。据报道：2011年我国因油气挥发而造成的经济损失高达47.6亿元^[2]。因此，控制汽油蒸汽类VOCs的排放、减少挥发油气损耗关系到环保、节能、安全和健康等诸多问题，也是政府和工业企业亟待解决的难题之一。中国在GB 31570-2015《石油炼制工业污染物排放标准》中对VOCs的排放做出了严格的规定：有机废气收集处理装置的排放气中非甲烷总烃含量不得高于60mg/m³，该标准将于2017年7月1日起执行^[3]。

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