Low-temperature SCR of NOx with NH3 over activated carbon fiber composite-supported metal oxides

Low-temperature SCR of NOx with NH3 over activated carbon fiber composite-supported metal oxides
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DOI:
10.1016/s0926-3373(02)00170-4
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发表时间:
2003-03
影响因子:
22.1
通讯作者:
G. Marbán;Raquel Antuña;A. B. Fuertes
G. Marbán;Raquel Antuña;A. B. Fuertes
中科院分区:
化学1区
文献类型:
--
作者:
G. Marbán;Raquel Antuña;A. B. Fuertes

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在以往的工作中,作者参与了Nomex基活性炭纤维(ACF)整体的制备和优化,并使用它们作为锰氧化物的催化剂载体的选择性催化还原(SCR)的NOx与NH3在低温下。因此,制造了由HNOMEX ™废弃物制成的低密度整料,并对其进行不同的表面调节处理,以使在SCR工艺中具有高活性的氧化锰的分散和负载最大化。为了完成这项研究,在这项工作中,使用不同的碳纤维来制造整体式载体,并分析衍生的氧化锰基催化剂的催化活性,并与标准Nomex™负载型催化剂的催化活性进行比较。这些纤维是煤沥青基、人造丝基、PAN基和酚醛树脂基碳纤维。此外,基于其他金属氧化物(镍、铬、钒和铁)的催化剂通过策略性改性的载体的平衡吸附(EA)和孔体积浸渍(PVI)来制备,以试图超越已经高度活性的基于氧化锰的催化剂的催化性能,并解决在实际条件下利用这些催化剂的主要缺点之一; SO2失活。对于所有制备的催化剂,在150°C的标准反应温度下评价以下参数:催化活性、选择性、载体气化程度、H2O抑制和SO2失活。此外,对特定样品进行了NO的程序升温脱附(TPD),以分析NO在催化剂表面的不同吸附模式。所有这些研究程序最终都是在催化剂(Nomex™废弃物基活性碳纤维复合材料(ACFC)负载的氧化铁)的选择中得出的,该催化剂构成了高催化性能和适度SO2失活之间的折衷。
In previous works, the authors were involved in the preparation and optimization of Nomex-based activated carbon fibers (ACFs) monoliths and their use as catalytic supports of manganese oxides for the selective catalytic reduction (SCR) of NOxwith NH3at low temperature. Thus, a low density monolith made of carbonized Nomex™ rejects was fabricated and submitted to different surface conditioning treatments in order to maximize the dispersion and loading of manganese oxides which were highly active in the SCR process. In order to complete the study, in this work different carbon fibers were used to fabricate the monolithic support, and the catalytic activity of the derived manganese oxide-based catalysts was analyzed and compared to that of the standard Nomex™-supported catalyst. These fibers were coal Pitch-, Rayon-, PAN-, and phenolic Resin-based carbon fibers. Additionally, catalysts based on other metal oxides (nickel, chromium, vanadium and iron) were prepared via equilibrium adsorption (EA) and pore volume impregnation (PVI) of the strategically modified supports, in an attempt to surpass the catalytic performance of the already highly active manganese oxide-based catalysts and to tackle one of the main drawbacks for the utilization of these catalysts under practical conditions; the SO2deactivation. For all the prepared catalysts the following parameters were evaluated at a standard reaction temperature of 150°C: catalytic activity, selectivity, extent of support gasification, H2O inhibition and SO2deactivation. Additionally temperature programmed desorption (TPD) of NO was conducted on specific samples in order to analyze the different adsorption modes of NO on the catalyst surface. All this research procedure has eventually derived in the selection of a catalyst (Nomex™ rejects-based activated carbon fiber composite (ACFC) supported iron oxides) which constitutes a compromise between high catalytic performance and moderate SO2deactivation.