水对V2O5 /AC低温催化NH3-SCR反应动力学的影响
首发时间:2012-04-13
摘要:活性炭担载五氧化二钒催化剂(V2O5/AC)在393-473K条件下对NH3-SCR反应具有良好的活性。但当烟气中含有水时其活性会降低。本文首先研究了水对该催化剂下本征动力学的影响。实验数据分别用机理模型(Eley-Rideal模型, Langmuir-Hinshelwood 模型和Mars-van Krevelen模型)和经验模型(一级反应模型和幂级数模型)进行拟合。结果显示,无论烟气中是否含有水,反应都遵循Eley-Rideal机理而不是Langmuir-Hinshelwood或Mars-van Krevelen机理;且随着水含量的增加,指前因子减小而活化能增大。最后,将得到的本征动力学模型参数代入到3D结构化反应器的数学模型之中,发现Eley-Rideal模型能更准确的描述反应器性能。
关键词: 本征动力学 选择性催化还原 V2O5/AC催化剂 结构化反应器 数学模型
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Influence of H2O on Kinetics of Low-Temperature SCR of NO by NH3 over V2O5 /AC Catalyst
Abstract:The AC (activated carbon) supported V2O5 (vanadium pentoxide) (V2O5/AC) catalyst shows high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) by ammonia (NH3) at 393-473 K after a pre-sulfated step. But the activities decrease obviously when adding H2O to the flue gas. The influence of H2O on intrinsic kinetics for this catalyst was first investigated in the absence of internal and external diffusions in a fixed-bed micro-reactor. Then, both the mechanical (i.e. Eley-Rideal model, Langmuir-Hinshelwood model, and Mars-van Krevelen model) and empirical (i.e. first-order model and power-rate law model) models were applied to correlate the experimental data. The results showed that the SCR of NO by NH3 over V2O5/AC catalyst follows the Eley-Rideal mechanism rather than Langmuir-Hinshelwood or Mars-van Krevelen mechanism whether H2O is contained in the flue gas or not, and the pre-exponential factor decreases and activation energy increases with the increasing amount of H2O. Finally, the intrinsic kinetic models obtained in this work were incorporated into a 3D mathematical model of monolithic reactor, and it was found that the Eley-Rideal model is more suitable for describing the SCR of NO by NH3 in the presence of H2O than the empirical models and thus should be adopted in the actual reactor design and scale-up for controlling the emission of NOx.
Keywords: Kinetics Selective catalytic reduction (SCR) V2O5/AC catalyst Monolithic reactor Mathematical model
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