SSZ-39 分子筛的合成原料配比及其脱硝催化性能

Synthesis raw material ratio and denitration catalytic performance of SSZ-39 zeolite

摘要

氨选择性催化还原(NH₃-SCR)是一种柴油机尾气高效净化技术。 SSZ-39 分子筛催化剂具备优良水热稳定性。 为降低其制备成本并提升催化活性，本文以低硅铝比Y 型分子筛为原料，通过转晶法合成 SSZ-39，系统考察碱金属、水、模板剂及晶种添加量对合成过程的影响，确定最优原料配比，再经离子交换得到多种过渡金属改性 SSZ-39 分子筛催化剂。 船舶工况模拟性能测试结果显示：相较 Fe-SSZ-39、Mn-SSZ-39，Cu-SSZ-39 具有更多可参与氧化还原循环的活性物种与丰富酸性位点，能够促进 Lewis 酸位点吸附的 NH₃ 还原 NO_x，表现出优异的 NH₃-SCR 催化性能，在 250℃～550℃区间， NO_x转化率可达 100％。

Abstract

Ammonia selective catalytic reduction (NH₃-SCR) is an efficient technology for diesel exhaust purification. SSZ-39 zeolite catalysts exhibit excellent hydrothermal stability. To reduce the preparation cost and improve catalytic activity, SSZ-39 was synthesized by interzeolite conversion by using low-silica Y zeolite as the starting material. The effects of alkali metal, water, template agent and seed crystal dosage on the synthesis process were systematically investigated, and the optimal raw material ratio was determined. A series of transition metal-modified SSZ-39 zeolite catalysts were then obtained via ion exchange. Performance tests under simulated marine operating conditions show that compared with Fe-SSZ-39 and Mn-SSZ-39, Cu-SSZ-39 possesses more redox-active species and abundant acid sites, which can promote the reduction of NO_x by NH₃ adsorbed on Lewis acid sites. Cu-SSZ-39 thus presents outstanding NH₃-SCR catalytic performance, with 100% NO_x conversion achieved in the temperature range of 250°C~550°C.

关键词

SSZ-39 分子筛 / 异晶转晶 / NH₃-SCR / 原料配比 / 脱硝性能

Key words

SSZ-39 zeolite / interzeolite conversion / NH₃-SCR / raw material ratio / NO_x removal performance

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基金资助

国家自然科学基金资助项目(22078037)

国家自然科学基金资助项目(52175378)

中央高校基本科研业务费专项资金资助项目(3132025221)