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1、湘潭大学 硕士学位论文 FeSO液相催化氧化脱硫及氨碱厂白泥盐泥海水浆液脱硫研 究 姓名：徐军科 申请学位级别：硕士 专业：环境工程 指导教师：童志权 20060501 I 摘 要 本文对 FeSO4液相催化氧化脱硫及氨碱厂白泥、盐泥海水浆液脱硫进行了研 究。 首先对活性炭及瓷拉西环两种填料用自来水进行脱硫对比实验，证明无论是 等宏观表面积还是等填料层高度，活性炭填料的脱硫率均高于瓷拉西环。然后在 活性炭填料塔中进行了 FeSO4液相催化氧化脱硫实验，考察了液气比、空塔气速、 吸收温度及 SO2进口浓度对脱硫率的影响。综合实验结果表明，连续运行 500 min 时，脱硫率及吸收液 pH 分别稳
2、定在 93.5%以上及 4.6 左右，且两者的变化趋势基 本一致。应用 MATLAB 计算机语言编程，拟合出脱硫率与各单因素之间的模拟 关系式：)/(5823. 7exp(00057259. 0 0072098. 00065149. 0011970. 00078910. 0 2 =tCGL so空 ，应用 该式计算出脱硫率的平均相对误差小于 5%，具有实际应用价值。 本项研究在烟气脱硫领域首次提出用具有较大比表面积的活性炭作填料，提 高了脱硫率，降低了运行费用，为我国开发从低浓度 SO2烟气中回收硫资源提供了 一种新的途径。 当前世界烟气脱硫仍以湿式石灰石/石灰抛弃法为主，脱硫剂石灰石/ 石灰
3、在脱硫成本中占有较大比重，而且这些脱硫剂的生产过程也造成一定的 环境污染。氨碱厂生产过程中产生的大量废渣（包括白泥和盐泥） ，由于得不到 充分的利用，绝大部分露天堆放，不仅占据着大量宝贵土地，还对环境造成了极 大的污染。受青岛碱厂的委托，本文对氨碱厂废渣作脱硫剂脱除烟气中 SO2进 行了系统的研究。 我国有不少氨碱厂位于海边，生产过程中大量使用海水，使用过的部分海水 排回大海。利用这些将排回大海的海水的天然碱度脱除烟气中 SO2，可以节约大量 淡水。但是，要维持较高的脱硫率必需消耗较大的动力。氨碱厂废渣含有大量的 碱性物质（碳酸钙、氧化钙或氢氧化镁等） ，加入海水（实验时，用海水素加水配 制而
4、成）中用来脱硫，直接或间接与烟气中的二氧化硫发生反应，可以达到提高 脱硫率、节支增效、双向治理、净化环境的目的。 首先用一次性脱硫工艺进行研究，单因素实验表明，液气比（L/G）对脱硫 率影响比较大。在实验条件范围内，SO2进口浓度及固含量对脱硫率的影响很小。 综合实验结果表明，无论是白泥还是盐泥海水浆液的脱硫率都很高，分别在 94%95%、95%97%之间。连续运行 16h 未观察到塔内有结垢现象，工业上可 以采用此工艺运行。但当浆液的固含量为 2%时，运行 3 小时后，塔内就出现 硬垢，因此该法只能在固含量很低（1%）的情况下运行。 上清液循环制浆脱硫工艺单因素实验表明， 在控制循环槽浆液
5、pH 值为 5.8 II 6.2 时，脱硫率随液气比的增加而增加，当白泥和盐泥浆液的液气比分别大于 5L/m 3、4L/m3 时，脱硫率均超过 96%。脱硫率随进口 SO2浓度的增大而明显下降。 由于上清液循环制浆时导致浆液中硫酸根离子的积累，从而加速了二水硫酸钙的 生成，致使设备结垢严重，工业上不能应用。 “钙-钙双碱法” 工艺单因素实验表明，液气比、进口 SO2浓度对脱硫率影 响比较大；循环浆液 pH 值小于 6.0 时影响较大，而大于 6.0 时影响相对较小；在 实验范围内，固含量对脱硫率影响较小。综合实验表明，在优化条件下，白泥、 盐泥浆液的脱硫率很高，分别平均为 95%和 96.9%
6、。连续运行 24h 后塔内有结垢 现象，但比上清液循环制浆脱硫法要好得多，采用此工艺能部分地防止塔内 结垢。 关键词: 关键词: 活性炭填料；硫酸亚铁；液相催化氧化；氨碱厂；白泥；盐泥；海水； 脱硫 III ABSTRACT Researches on Desulphurization by FeSO4 Aqueous Catalytic Oxidation and by using the Serosity of White Sludge or Salt Sludge of Ammonia Alkali Mills were studied. Contrastive experiments
7、of desulphurization by tap water with active carbon and porcelain Raschig ring fillers were studied. The results indicated that SO2 removal efficiency with active carbon as filler was better than that with porcelain Raschig ring as filler, whether their macroscopic surface areas or heights were equa
8、l. Then the experiment of desulphurization by FeSO4 aqueous catalytic oxidation in active carbon tower was studied, and the effect of liquid-gas ratio, superficial gas flow rate, absorption temperature and inlet concentration of SO2 was studied too. The synthesis experiment showed that desulphurizat
9、ion efficiency and absorbent pH could keep up more than 93.5% and about 4.6 respectively after 500 minutes continuous run. The change trend of desulphurization efficiency and absorbent pH was consistent basically. Using MATLAB compute language programme, the equation of simulation relation between d
10、esulphurization efficiency and all factors was drawn up: )/(5823. 7exp(00057259. 0 0072098. 00065149. 0011970. 00078910. 0 2 =tCGL so空 .The average relative error which was caused from computing with this equation was less than 5%. Using activated carbon with greater comparative surface-area as fill
11、er was put forward for the first time in the field of flue gas desulphurization in this research. As this, it could advance desulphurization efficiency and reduce running fee. It provided a new approach of reclaiming sulfur resource from flue gas with low concentration SO2 for our national research.
12、 At present, the method of wet lime stone / lime abandon is the main flue gas desulphurization technology in the world. The desulfurizer lime stone/lime occupies greater specific gravity in the desulphurization cost. And in the production process of desulfurizer, it will cause certain environmental
13、pollution too. During the production in ammonia alkali factory, it produced a great deal of waste sediment (containing white sludge and salt sludge) which was mostly piled up on the ground because of not being used abundantly. As this, not only occupied it plenty of valuable earth, but also brought
14、about infinite pollution. Entrusted by Qingdao Alkali Factory, the systematic investigation of taking off SO2 from flue gas with the waste sediment of ammonia IV alkali factory as desulfurizer was carried for the first time. In our country, there are many ammonia alkali factories which locate near s
15、easide and use a great deal of seawater, part of which must be discharged into sea, in the process of production. It can save plenty of fresh water, using these natural alkali matters contained in the seawater being to be discharged into sea to remove SO2 from flue gas. But, it need consume more pow
16、er for maintaining better desulphurization efficiency. The waste sediment of ammonia alkali factory contains many alkali matters (CaCO3、Ca(OH)2、Mg(OH)2) which can be entered into seawater (in experiment, confect using seawater salt and tap water ) to remove SO2. These alkali matters can occur neutralization reaction with SO2 contained in flue gas directly or indirectly, which c
