4.8 Article

Rational Regulation of Reducibility and Acid Site on Mn-Fe-BTC to Achieve High Low-Temperature Catalytic Denitration Performance

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c20545

Keywords

nitrogen oxide; metal organic framework; reducibility; acid site; DFT calculation

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Selective catalytic reduction with ammonia is the mainstream technology for flue gas denitration. The reducibility and acid site are two important factors affecting de-NOx performance, and their regulation through synthesis of Mn-Fe-BTC catalyst with different ratios of Mn and Fe has been investigated. The research provides guidance for flexible regulation of reducibility and acid site of low-temperature de-NOx catalyst.
Selective catalytic reduction with ammonia is the mainstream technology of flue gas denitration (de-NOx). The reducibility and acid site are two important factors affecting the de-NOx performance, and effective regulation between them is the key to obtain a highly efficient de-NOx catalyst. Herein, a series of Mn-Fe-BTC with different ratios of Mn and Fe are synthesized, among which 2Mn-1Fe-BTC with 2:1 molar ratio of Mn and Fe has excellent low-temperature (LT) de-NOx performance (above 90% NO conversion between 60 and 270 degrees C) and good tolerance to H2O and SO2 poisoning (88% NO conversion at 150 degrees C with 100 ppm of SO2 and/or 6% H2O). It is revealed that the reducibility properties and acid sites of Mn-Fe- BTC can be flexibly tuned by the ratio of Mn and Fe. The difference in electronegativity between Fe and Mn leads to the redistribution of valence electrons, which enables the controllable reducibility of Mn-Fe-BTC. Furthermore, different amounts of Mn and Fe lead to different electron transport, which determines the type and number of acid sites. The synergistic effect of Mn and Fe endows Mn-Fe-BTC with enhanced surface molecular adsorption capacity and enables the catalyst to selectively chemisorb NH3 and NO at different active sites. This research provides guidance for the flexible regulation of reducibility and acid site of LT de-NOx catalyst.

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