Formation and Effect of NH4+ Intermediates in NH3-SCR over Fe-ZSM-5 Zeolite Catalysts

被引：80

作者：

Chen, Peirong ^{[1
,2
]}

Jablonska, Magdalena ^{[2
,3
]}

Weide, Philipp ^{[4
]}

Caumanns, Tobias ^{[5
]}

Weirich, Thomas ^{[2
,5
]}

Muhler, Martin ^{[4
]}

Moos, Ralf ^{[6
,7
]}

Palkovits, Regina ^{[2
,3
]}

Simon, Ulrich ^{[1
,2
]}

机构：

[1] Rhein Westfal TH Aachen, Inst Inorgan Chem, Landoltweg 1, D-52074 Aachen, Germany

[2] Rhein Westfal TH Aachen, Ctr Automot Catalyt Syst Aachen, Aachen, Germany

[3] Rhein Westfal TH Aachen, Chair Heterogeneous Catalysis & Chem Technol, Worringerweg 2, D-52074 Aachen, Germany

[4] Ruhr Univ Bochum, Lab Ind Chem, D-44780 Bochum, Germany

[5] Rhein Westfal TH Aachen, Cent Facil Electron Microscopy, D-52074 Aachen, Germany

[6] Univ Bayreuth, Bayreuth Engine Res Ctr, Dept Funct Mat, Univ Str 30, D-95440 Bayreuth, Germany

[7] Univ Bayreuth, Zentrum Energietech, Univ Str 30, D-95440 Bayreuth, Germany

来源：

ACS CATALYSIS | 2016年 / 6卷 / 11期

关键词：

ammonium ion intermediates; NO activation; proton transport; redox cycle; NH3-SCR mechanism; ACTIVE-SITES; SELECTIVE REDUCTION; DENO(X) CATALYSTS; NITROGEN-OXIDES; NOX; IRON; SPECTROSCOPY; CONVERSION; IMPEDANCE; INSIGHTS;

D O I：

10.1021/acscatal.6b02496

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：

With the help of a technique combining in situ electrical impedance spectroscopy and DRIFT spectroscopy, we observed directly the formation of ammonium ion (NH4+) intermediates resulting from the interaction of NO and NH3 on Fe-ZSM-5 catalysts for selective catalytic reduction by NH3 (NH3-SCR). The formed NH4+ intermediates, indicating the activation of NO in the presence of adsorbed NH3, were found to be strongly related to the NH3-SCR activity of Fe-ZSM-5 catalysts at low temperatures. These findings, which are not easily achievable by conventional methods, provide new and important perspectives to understand mechanistically the NH3-SCR reaction over Fe-zeolite catalysts.

引用

页码：7696 / 7700

页数：5

共 36 条

[1] Methods for NH3 titration of Bronsted acid sites in Cu-zeolites that catalyze the selective catalytic reduction of NOx with NH3 [J].

Bates, Shane A. ;

Delgass, W. Nicholas ;

Ribeiro, Fabio H. ;

Miller, Jeffrey T. ;

Gounder, Rajamani .

JOURNAL OF CATALYSIS, 2014, 312 :26-36

[2] Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials [J].

Beale, A. M. ;

Gao, F. ;

Lezcano-Gonzalez, I. ;

Peden, C. H. F. ;

Szanyi, J. .

CHEMICAL SOCIETY REVIEWS, 2015, 44 (20) :7371-7405

[3] Selective Catalytic Reduction of NO Over Fe-ZSM-5: Mechanistic Insights by Operando HERFD-XANES and Valence-to-Core X-ray Emission Spectroscopy [J].

Boubnov, Alexey ;

Carvalho, Hudson W. P. ;

Doronkin, Dmitry E. ;

Guenter, Tobias ;

Gallo, Erik ;

Atkins, Andrew J. ;

Jacob, Christoph R. ;

Grunwaldt, Jan-Dierk .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (37) :13006-13015

[4] The determination of the activities of different iron species in Fe-ZSM-5 for SCR of NO by NH3 [J].

Brandenberger, Sandro ;

Kroecher, Oliver ;

Tissler, Arno ;

Althoff, Roderik .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 95 (3-4) :348-357

[5] The role of Bronsted acidity in the selective catalytic reduction of NO with ammonia over Fe-ZSM-5 [J].

Brandenberger, Sandro ;

Kroecher, Oliver ;

Wokaun, Alexander ;

Tissler, Arno ;

Althoff, Roderik .

JOURNAL OF CATALYSIS, 2009, 268 (02) :297-306

[6] The State of the Art in Selective Catalytic Reduction of NOx by Ammonia Using Metal-Exchanged Zeolite Catalysts [J].

Brandenberger, Sandro ;

Kroecher, Oliver ;

Tissler, Arno ;

Althoff, Roderik .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2008, 50 (04) :492-531

[7] Monitoring NH3 storage and conversion in Cu-ZSM-5 and Cu-SAPO-34 catalysts for NH3-SCR by simultaneous impedance and DRIFT spectroscopy [J].

Chen, Peirong ;

Simboeck, Johannes ;

Schoenebaum, Simon ;

Rauch, Dieter ;

Simons, Thomas ;

Palkovits, Regina ;

Moos, Ralf ;

Simon, Ulrich .

SENSORS AND ACTUATORS B-CHEMICAL, 2016, 236 :1075-1082

[8] The effect of Cu and Fe cations on NH3-supported proton transport in DeNOx-SCR zeolite catalysts [J].

Chen, Peirong ;

Rauch, Dieter ;

Weide, Philipp ;

Schoenebaum, Simon ;

Simons, Thomas ;

Muhler, Martin ;

Moos, Ralf ;

Simon, Ulrich .

CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (10) :3362-3366

[9] Correlating the Integral Sensing Properties of Zeolites with Molecular Processes by Combining Broadband Impedance and DRIFT Spectroscopy-A New Approach for Bridging the Scales [J].

Chen, Peirong ;

Schoenebaum, Simon ;

Simons, Thomas ;

Rauch, Dieter ;

Dietrich, Markus ;

Moos, Ralf ;

Simon, Ulrich .

SENSORS, 2015, 15 (11) :28915-28941

[10] A comparative study of the NH3-SCR reactions over a Cu-zeolite and a Fe-zeolite catalyst [J].

Colombo, Massimo ;

Nova, Isabella ;

Tronconi, Enrico .

CATALYSIS TODAY, 2010, 151 (3-4) :223-230

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