| 徐国强,苏亚欣,温妮妮,张恒,刘权,邓文义,周皞.Ti-PILC负载Ga-Fe的CH4-SCR脱硝性能研究[J].分子催化,2022,36(4):347-359 |
| Ti-PILC负载Ga-Fe的CH4-SCR脱硝性能研究 |
| Study on CH4-SCR Performance by Ga-Fe Catalysts Supported on Ti-pillared Interlayered Clays (Ti-PILC) |
| 投稿时间：2022-05-05 修订日期：2022-05-31 |
| DOI：10.16084/j.issn1001-3555.2022.04.006 |
| 中文关键词: NOx脱除 CH4-SCR Ti-PILC 抗水蒸气 抗SO2 |
| 英文关键词:NOx removal CH4-SCR Ti-PILC water vapor resistance SO2 resistance |
| 基金项目:国家自然科学基金项目(No. 52276103); 上海市自然科学基金项目(No.19ZR1400700, 17ZR1419300)；江苏省自然科学基金(No.BK20181161) |
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| 中文摘要: |
| 为解决柱撑粘土(PILC)系催化剂在CH4作还原剂条件下选择性催化还原(SCR: selective catalytic reduction)NO效率较低、抗水蒸气、抗SO2毒化能力较差等问题, 提出了一种较为新颖的催化剂制备方法. 利用TiCl4作为Ti源对Na化蒙脱土进行柱撑得到Ti-PILC, 之后以浸渍法和离子交换法分别负载活性金属Ga和Fe得到xGa/Ti-PILC系列和yFe-14Ga/Ti-PILC系列催化剂. 采用多种方法对催化剂的基础物理化学性质进行了表征, 并在固定床微反应器上进行了CH4-SCR脱硝实验. 结果表明, 14Ga/Ti-PILC于500 ℃达到了77%的NO还原率, 引入Fe后, 催化剂的抗水抗硫性能得到了提高, 如10Fe-14Ga/Ti-PILC, 在含5%水蒸气和0.02%SO2条件下, NO脱除效率下降不超过10%和8%. 对催化剂进行N2吸附-脱附、H2-TPR、XRD、XPS、UV-vis、Py-FTIR等相关表征及分析后发现: Ga在Ti-PILC上分散度较高的情况下能有效提升催化剂对NO的还原性能; 通过引入适量的Fe增加14Ga/Ti-PILC的孔径从而可较为有效地降低水蒸气和SO2对催化剂脱硝活性的负面影响; 催化剂表面存在的Lewis酸的含量与催化剂的脱硝活性呈正相关关系. |
| 英文摘要: |
| In order to solve the problems associated with the selective catalytic reduction (SCR) of NO by CH4, such as low efficiency, poor resistance to water vapor and SO2 poisoning, a novel catalyst preparation method was proposed. TiCl4 was used as Ti precursor to pillar the Na-montmorillonite and prepare the Ti-pillared layered clays (Ti-PILC), and then the active metals Ga and Fe were loaded by impregnation and ion exchange methods respectively to obtain xGa/Ti-PILC and yFe-14Ga/Ti-PILC series catalysts. Several techniques were used to character the basic chemical and physical properties of the catalysts and the SCR of NO with CH4 as the reducing agent was tested in a fixed-bed micro-reactor. The results showed that, among all the catalysts, the NO reduction rate by 14Ga/Ti-PILC reached 77% at 500 ℃. When Fe was loaded on and the 14Ga/Ti-PILC, the resistance to both water vapor and SO2 were improved, e.g., less than 10% and 8% decreases of the NO reduction were tested for 10Fe-14Ga/Ti-PILC catalyst under the condition of 5% water vapor and 0.02% SO2. The characterization results of the catalysts, such as N2 adsorption desorption, H2-TPR, XRD, XPS, UV-vis and Py-FTIR, showed that Ga can effectively improve the NO reduction when the Ga was highly dispersed on the Ti-PILC surface. Introducing an appropriate amount of Fe could increase the pore size of 14Ga/Ti-PILC and then the negative effects of water vapor and SO2 on the SCR activity could be effectively reduced. The content of Lewis acid on the catalyst surface is positively correlated with the SCR activity of the catalyst. |
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