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N2O inhibition by toluene over Mn-Fe spinel SCR catalyst
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-02-19 , DOI: 10.1016/j.jhazmat.2021.125468
Peng Lu , Lyumeng Ye , Xianhui Yan , Xiongbo Chen , Ping Fang , Dongyao Chen , Dingsheng Chen , Chaoping Cen

Co-removal of toluene in NH3-SCR unit over Mn based catalysts is desirable but still faces the big challenge of byproduct greenhouse gas N2O. In this work, the impacts of toluene on N2O formation mechanism was studied. The main N2O formation pathways in NH3-SCR over Mn-Fe spinel were NH3 oxidation and non-catalytic selective reduction (NSCR), in which NSCR dominated below 250 °C. The N2O from NSCR through both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms was confirmed. And the E-R mechanism was dominant at 200 °C. Toluene was effectively co-removed with NOx with the advantage of N2O inhibition. Toluene suppressed N2O generation from both NH3 oxidation and NSCR. NH3 oxidation by gaseous O2 and catalyst surface oxygen was all limited by toluene, resulting in less adsorbed NH that was further proved by the larger energy barriers of NH3*→NH2* and NH2*→NH* on toluene pre-adsorbed catalyst surface. NO oxidation was also limited, suppressing the generation of adsorbed NO3. Due to the inhibition of NH3 and NO activation to key intermediates NH and NO3, respectively, the N2O generation from E-R route was slightly decreased in the presence of toluene, while that from L-H route was completely prohibited at 200 °C.



中文翻译:

Mn-Fe尖晶石SCR催化剂上甲苯对N 2 O的抑制作用

在NH 3 -SCR单元中通过Mn基催化剂共除去甲苯是理想的,但仍然面临着副产物温室气体N 2 O的巨大挑战。在这项工作中,研究了甲苯对N 2 O形成机理的影响。Mn-Fe尖晶石上NH 3 -SCR中主要的N 2 O形成途径为NH 3氧化和非催化选择性还原(NSCR),其中NSCR在250°C以下占主导地位。确认了来自NSCR的N 2 O通过Eley-Rideal(ER)和Langmuir-Hinshelwood(LH)机制。ER机制在200°C时占主导地位。借助N 2可以有效地将甲苯与NO x共同脱除O抑制。甲苯抑制Ñ 2从两个NH阿代3氧化和NSCR。气态O 2和催化剂表面氧对NH 3的氧化均受甲苯的限制,从而减少了NH的吸附,这进一步得到了NH 3 *→NH 2 *和NH 2 *→NH *在甲苯预分离塔上的较大能垒的进一步证明。吸附的催化剂表面。NO氧化反应也受到限制,从而抑制吸附NO的产生3 - 。由于NH的抑制3和NO激活到关键中间体NH和NO 3 - ,分别,将N 2在甲苯存在下,ER途径的O生成量略有减少,而LH途径的O生成在200°C时被完全禁止。

更新日期:2021-02-28
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