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Er composition (X)-mediated catalytic properties of Ce1-XErXVO4 surfaces for selective catalytic NOX reduction with NH3 at elevated temperatures

期刊

CATALYSIS TODAY
卷 359, 期 -, 页码 65-75

出版社

ELSEVIER
DOI: 10.1016/j.cattod.2019.05.030

关键词

CeVO4; ErVO4; Ce1-XErXVO4; Selective catalytic NOX reduction; NH3 oxidation; Hydro-thermal aging

资金

  1. Ministry of Science and ICT of South Korea [NRF-2017M3D1A1040690]
  2. Korea Institute of Science and Technology (KIST) [2E29250]
  3. National Research Foundation of Korea [2E31210, 2017M3D1A1040690] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Rare earth metal vanadates have shown promise for converting NOX to N-2 at high temperatures, but face limitations in catalytic activity due to weak hydrothermal stability, low N-2 selectivity, and limited active sites. This study demonstrates the efficacy of structurally modifying vanadate with additional rare earth metals to generate bimetallic vanadates with improved reactivity and stability.
Catalytic rare earth metal vanadates have shown promise for efficiently converting NOX to N-2 at elevated temperatures (NH3-SCR) (e.g., CeVO4, ErVO4, and TbVO4). However, these vanadates have limitations as cata-lytic sites because of three major issues such as weak hydro-thermal stability, low N-2 selectivity, and limited numbers of major active (Lewis acid) sites. As an efficient way to circumvent these constraints, this study showcases a means of structurally modifying vanadate with additional rare earth metals to generate bimetallic vanadates with variable metal compositions. While selecting Ce and Er as metal constituents, a series of Ce1-XErXVO4 solid solutions were deposited onto WO3-promoted TiO2 supports (WO3-TiO2) to form ErX catalysts, whereas a control simulating a commercial catalyst (V) was also synthesized using WO3-TiO2 for comparison. Bimetallic Ce1-XErXVO4 (X = 0.25, 0.5, and 0.75) showed enhanced redox features, improved the quantities of Lewis/Bronsted acid sites and defects, and increased resistance to hydro-thermal aging relative to their monometallic analogues (X = 0 and 1). The optimal Er composition of Ce1-XErXVO4 studied was found to be X = 0.5. This was because Er-0.5 provided the best redox character, the largest number of active sites with the desired Lewis acid strength, and the greatest hydro-thermal stability among all the ErX and V catalysts studied. This led to the best catalytic consequence of Er-0.5 in the selective NH3 oxidation and the NH3-SCR reactions, both of which should achieve high N-2 productivities at elevated temperatures. In addition, Er-0.5 subjected to hydro thermal aging also extended its best NH3-SCR performance among all aged catalysts studied even to low temperature regime of < 300 degrees C. This paper remarks the proper combination of rare earth metals used to construct bimetallic vanadates can be adaptable to create high-performance NH3-SCR catalysts for use at elevated temperatures.

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