NO reduction with H2 in the presence of excess O2 over Pd/MFI catalyst

NO reduction with H2 in the presence of excess O2 over Pd/MFI catalyst
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DOI:
10.1016/s0016-2361(02)00141-2
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发表时间:
2002-09
期刊:
影响因子:
7.4
通讯作者:
Bin Wen
Bin Wen
中科院分区:
工程技术1区
文献类型:
--
作者:
Bin Wen

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研究了升华法制备的 Pd/MFI 催化剂在过量 O2 存在下与 H2 的 NO SCR(选择性催化还原)活性。当 GHSV=90 000h−1 时,NO 在 100°C 时达到非常高的稳态转化为 N2 (70%)。当催化剂在反应温度下首次与所有反应物和产物接触时,催化剂内部会发生显着的重组。 Pd0 在 NO-H2-O2 反应中起重要作用,可能是 NO 还原的活性位点。 Pd-β氢化物的形成使NO还原催化剂失活。在整个NO-H2-O2反应中,没有N2O或NO2形成; N2是唯一的含氮产品。 O2 的存在抑制了不需要的 NH3 的形成。 NO+H2反应的速率快或与H2+O2反应的速率相当。 PdO 的氧化和随后的 PdO 团聚是高温下 NO 还原活性降低的原因。
The NO SCR (selective catalytic reduction) activity with H2in the presence of excess O2was investigated over Pd/MFI catalyst prepared by sublimation method. With GHSV=90 000h−1, a very high steady-state conversion of NO to N2(70%) is achieved at 100°C. Significant reorganizations take place inside the catalyst upon its first contact with all reactants and products at the reaction temperature. Pd0, which has a significant role in the NO–H2–O2reaction, is possibly the active site for NO reduction. The formation of Pd-β hydride deactivates the catalyst for NO reduction. Throughout the entire NO–H2–O2reaction, no N2O or NO2is formed; N2is the only N-containing product. The presence of O2inhibits the formation of undesirable NH3. The rate of the NO+H2reaction is fast or comparable to that of the H2+O2reaction. The oxidation of Pd0and subsequent agglomeration of PdO are responsible for the decreased NO reduction activity at high temperature.