Rational selection of Fe2V4O13 over FeVO4 as a preferred active site on Sb-promoted TiO2 for catalytic NOX reduction with NH3

被引:41
作者
Kim, Jongsik [1 ]
Kim, Dong Ho [1 ]
Kwon, Dong Wook [1 ]
Ha, Heon Phil [1 ,2 ]
机构
[1] Korea Inst Sci & Technol, Mat Architecturing Res Ctr, Seoul 02792, South Korea
[2] Univ Sci & Technol, Dept Nanomat Sci & Engn, Daejeon 34113, South Korea
基金
新加坡国家研究基金会;
关键词
AMMONIUM BISULFATE FORMATION; VANADIUM-OXIDE CATALYSTS; LOW-TEMPERATURE SCR; VANADATE CATALYSTS; PERFORMANCE; V2O5/TIO2; MECHANISM; CERIA; DECOMPOSITION; RESISTANCE;
D O I
10.1039/c8cy01304g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
FeVO4 (Fe-1) is a particular class of metal vanadate that has recently been highly profiled as an active site to selectively reduce NOX with NH3 (NH3-SCR). This primarily results from NOX/NH3-accessible VO43- anions and an electronic inductive effect between the Fe and V species, leading to the formation of abundant catalytic defects available for NOX turnover. Motivated by a structural inspection of the vanadates reported to date, this study detailed the use of Fe2V4O13 (Fe-2) as a novel active site deposited on anatase (TiO2) for NH3-SCR. While providing the aforementioned structural benefits, Fe-2/TiO2 also enhanced the redox character as well as the number of sites accessible to NOX/NH3 over Fe-1/TiO2 because of the greater electronic inductive effect of Fe-2. Therefore, Fe-2/TiO2 converted NOX better than Fe-1/TiO2 in the presence of H2O. To further improve the NH3-SCR performance of Fe-2/TiO2, its catalytic surface was modified via two steps. The first step was to incorporate 1.9 wt% Sb into Fe-2/TiO2. Sb could promote the redox feature of Fe-2/TiO2 and help its surface to preferentially interact with NH3/NOX, thereby making the resulting Fe-2-Sb-1.9/TiO2 outperform Fe-2/TiO2 during NH3-SCR in the presence of H2O. The second step was to functionalize the Fe-2-Sb-1.9/TiO2 surface with SO32-/SO42- species. The resulting Fe-2-Sb-1.9/TiO2 (S) was validated to further increase redox cycling of Fe-2-Sb-1.9/TiO2, favor NO2 production from NO oxidation for fast NH3-SCR, and hamper surface interplay with SO2. Fe-2-Sb-1.9/TiO2 (S), therefore, showed higher NOX conversions than a control simulating a commercial catalyst during NH3-SCR feeding H2O and SO2. Fe-2-Sb-1.9/TiO2 (S) also showed greater durability than the control because of its enhanced resistance to SO2, ammonium (bi)sulfates, and alkali metals.
引用
收藏
页码:4774 / 4787
页数:14
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