<br>用于 NOx CH4-SCR 的工程 In-Co3O4/H-SSZ-39(OA) 催化剂：温和草酸 (OA) 浸出和 Co3O4 改性,Molecules

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用于 NOx CH4-SCR 的工程 In-Co3O4/H-SSZ-39(OA) 催化剂：温和草酸 (OA) 浸出和 Co3O4 改性
Molecules ( IF 4.2 ) Pub Date : 2024-08-07 , DOI: 10.3390/molecules29163747
Guanyu Chen ₁ , Weixin Zhang ₁ , Rongshu Zhu ₁ , Yanpeng Chen ₁ , Minghu Zhao ₁ , Mei Hong ₂

Affiliation

沸石基催化剂可有效催化甲烷选择性催化还原氮氧化物 (CH4-SCR)，以环境友好的方式去除氮氧化物，但在含 SO2 和 H2O 的高温烟气中会严重失活。在这项工作中，报道了具有高水热稳定性的SSZ-39沸石（AEI拓扑）用于制备CH4-SCR催化剂。用草酸（OA）进行弱酸浸不仅将商用SSZ-39的Si/Al比调节到合适的值，而且还去除了一些骨架外的Al原子，在沸石中引入了少量介孔，减轻了扩散限制。铟交换过程中额外的 Co3O4 修饰进一步增强了所得 In-Co3O4/H-SSZ-39(OA) 的催化活性。优化后的样品在气时空速 (GHSV) 为 24,000 h−1 且存在 5 vol% H2O 的情况下在 CH4-SCR 中表现出卓越的性能。即使在严酷的含SO2和H2O的高温条件下，它也表现出令人满意的稳定性。含有 Co3O4 组分的催化剂表现出更高的 CH4 转化率。通过 NO (NO-TPD) 的程序升温脱附证实，Co3O4 和 Brønsted 酸位之间的强相互作用使得 In-Co3O4/H-SSZ-39(OA) 中保留更稳定的 NxOy 物质，以进一步提供高温下发生反应。

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Engineering In-Co3O4/H-SSZ-39(OA) Catalyst for CH4-SCR of NOx: Mild Oxalic Acid (OA) Leaching and Co3O4 Modification

Zeolite-based catalysts efficiently catalyze the selective catalytic reduction of NOx with methane (CH4-SCR) for the environmentally friendly removal of nitrogen oxides, but suffer severe deactivation in high-temperature SO2- and H2O-containing flue gas. In this work, SSZ-39 zeolite (AEI topology) with high hydrothermal stability is reported for preparing CH4-SCR catalysts. Mild acid leaching with oxalic acid (OA) not only modulates the Si/Al ratio of commercial SSZ-39 to a suitable value, but also removes some extra-framework Al atoms, introducing a small number of mesopores into the zeolite that alleviate diffusion limitation. Additional Co3O4 modification during indium exchange further enhances the catalytic activity of the resulting In-Co3O4/H-SSZ-39(OA). The optimized sample exhibits remarkable performance in CH4-SCR under a gas hourly space velocity (GHSV) of 24,000 h−1 and in the presence of 5 vol% H2O. Even under harsh SO2- and H2O-containing high-temperature conditions, it shows satisfactory stability. Catalysts containing Co3O4 components demonstrate much higher CH4 conversion. The strong mutual interaction between Co3O4 and Brønsted acid sites, confirmed by the temperature-programmed desorption of NO (NO-TPD), enables more stable NxOy species to be retained in In-Co3O4/H-SSZ-39(OA) to supply further reactions at high temperatures.

更新日期：2024-08-08

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