Supporting Information Generation of NH3 Selective Catalytic ...
Supporting Information
Generation of NH3 Selective Catalytic Reduction Active Catalysts from Decomposition of Supported FeVO4 Adrian Marberger,†,‡ Martin Elsener,† Davide Ferri,† Amod Sagar,¶ Karl Schermanz,¶ and Oliver Kr¨ocher∗,†,‡ †Paul Scherrer Institut, CH-5232 Villigen, Switzerland ´ ‡Ecole Polytechnique F´ed´erale de Lausanne (EPFL), Institute of Chemical Science and Engineering, CH-1015 Lausanne, Switzerland ¶Department of Chemistry R&D, Treibacher Industrie AG, A-9330 Althofen, Austria E-mail: [email protected] Phone: +4156 310 20 66
S1
Supporting Information
Figure S1 displays the Arrhenius plot of the kmass of FeVTWS-550, FeVTWS-650 and reference material VTWS-650. In Figure S1a, it is evident that the Arrhenius plot of the kmass is only linear up to a reaction temperature of 300
. Above that temperature, various
effects such as internal and external mass transfer limitations prevent the use of these kmass for an linear regression (Fig. S1b).
Arrhenius Plot
7
7
FeVTWS-550
Activation Energy
FeVTWS-650
(kJ/mol)
VTWS-650 6
FeVTW S-550 FeVTW S-650 VTW S-650
62.2 +/- 0.2
Linear Regression
60.9 +/- 0.5
6
Linear Regression
350°C
Linear Regression
mass
300°C
ln(k
ln(k
300°C
)
5
mass
)
5
4
4
50.9 +/- 3.7 250°C
250°C 3
3
200°C
200°C 2
2
0.0012
0.0013
0.0014
0.0015
0.0016
0.0017
1/T (1/°C)
0.0018
0.0019
0.0020
0.0016
0.0021
0.0017
0.0018
0.0019
1/T (1/°C)
(a) Temperature range: 200 - 550
0.0020
0.0021
(b) Temperature range: 200 - 300
Figure S1: Arrhenius plot of the kmass at 200, 250 and 300 and VTWS-650.
S2
of FeVTWS-550, FeVTWS-650
Figure S2 is showing the DeNOx performance of the reference material VTWS calcined at various temperatures.
100
500
(a)
Rate at 250°C
(b)
Rate at 300°C
400
60
VTW S - 550°C
40
VTW S - 600°C
VTW S - 700°C DeNOx at 10 ppm NH3
20
200
mass
VTW S - 650°C
300
k
DeNOx / %
3
NO - SCR [cm /(g*s)]
80
100
DeNOx at 10 ppm NH3 DeNOx at 10 ppm NH3 DeNOx at 10 ppm NH3 0
0 200
250
300
350
400
450
500
550
Temperature / °C
550 550
600 600
650 650
700 700
Calcination Temp. / °C
Figure S2: a) DeNOx activity of 2.3 wt% V2 O5 /TWS calcined at 550 , 600 , 650 and 700 for 10 h. Reaction conditions: 0 - 600 ppm NH3 , 500 ppm NO, 10 vol% O2 , 5 vol% H2 O (bal. N2 ), GHSV: 50 000 h−1 . b) Mass specific rate constants (kmass ) as function of calcination temperature of VTWS.
S3
Figure S3 is showing the N2 O production of the catalysts from Fig. 3, 4.5FeVTWS calcined at 550 - 700
as well as the reference material VTWS-650.
50 48
maximal N O 2
4.5FeVTW S-550
46
4.5FeVTW S-600 4.5FeVTW S-650 4.5FeVTW S-700
30
N2O / ppm
VTW S-650
N O at 10 ppm NH 2
20
3
slip
4.5FeVTW S-550 4.5FeVTW S-600 4.5FeVTW S-650
10
4.5FeVTW S-700 VTW S-650
0 200
250
300
350
400
450
500
550
Temperature / °C
Figure S3: a) N2 O production of 4.5FeVTWS calcined at 550 , 600 , 650 and 700 for 10 h. Reaction conditions: 0 - 600 ppm NH3 , 500 ppm NO, 10 vol% O2 , 5 vol% H2 O (bal. N2 ), GHSV: 50 000 h−1 .
S4
Generation of NH3 Selective Catalytic Reduction Active Catalysts from Decomposition of Supported FeVO4 Adrian Marberger,†,‡ Martin Elsener,† Davide Ferri,† Amod Sagar,¶ Karl Schermanz,¶ and Oliver Kr¨ocher∗,†,‡ †Paul Scherrer Institut, CH-5232 Villigen, Switzerland ´ ‡Ecole Polytechnique F´ed´erale de Lausanne (EPFL), Institute of Chemical Science and Engineering, CH-1015 Lausanne, Switzerland ¶Department of Chemistry R&D, Treibacher Industrie AG, A-9330 Althofen, Austria E-mail: [email protected] Phone: +4156 310 20 66
S1
Supporting Information
Figure S1 displays the Arrhenius plot of the kmass of FeVTWS-550, FeVTWS-650 and reference material VTWS-650. In Figure S1a, it is evident that the Arrhenius plot of the kmass is only linear up to a reaction temperature of 300
. Above that temperature, various
effects such as internal and external mass transfer limitations prevent the use of these kmass for an linear regression (Fig. S1b).
Arrhenius Plot
7
7
FeVTWS-550
Activation Energy
FeVTWS-650
(kJ/mol)
VTWS-650 6
FeVTW S-550 FeVTW S-650 VTW S-650
62.2 +/- 0.2
Linear Regression
60.9 +/- 0.5
6
Linear Regression
350°C
Linear Regression
mass
300°C
ln(k
ln(k
300°C
)
5
mass
)
5
4
4
50.9 +/- 3.7 250°C
250°C 3
3
200°C
200°C 2
2
0.0012
0.0013
0.0014
0.0015
0.0016
0.0017
1/T (1/°C)
0.0018
0.0019
0.0020
0.0016
0.0021
0.0017
0.0018
0.0019
1/T (1/°C)
(a) Temperature range: 200 - 550
0.0020
0.0021
(b) Temperature range: 200 - 300
Figure S1: Arrhenius plot of the kmass at 200, 250 and 300 and VTWS-650.
S2
of FeVTWS-550, FeVTWS-650
Figure S2 is showing the DeNOx performance of the reference material VTWS calcined at various temperatures.
100
500
(a)
Rate at 250°C
(b)
Rate at 300°C
400
60
VTW S - 550°C
40
VTW S - 600°C
VTW S - 700°C DeNOx at 10 ppm NH3
20
200
mass
VTW S - 650°C
300
k
DeNOx / %
3
NO - SCR [cm /(g*s)]
80
100
DeNOx at 10 ppm NH3 DeNOx at 10 ppm NH3 DeNOx at 10 ppm NH3 0
0 200
250
300
350
400
450
500
550
Temperature / °C
550 550
600 600
650 650
700 700
Calcination Temp. / °C
Figure S2: a) DeNOx activity of 2.3 wt% V2 O5 /TWS calcined at 550 , 600 , 650 and 700 for 10 h. Reaction conditions: 0 - 600 ppm NH3 , 500 ppm NO, 10 vol% O2 , 5 vol% H2 O (bal. N2 ), GHSV: 50 000 h−1 . b) Mass specific rate constants (kmass ) as function of calcination temperature of VTWS.
S3
Figure S3 is showing the N2 O production of the catalysts from Fig. 3, 4.5FeVTWS calcined at 550 - 700
as well as the reference material VTWS-650.
50 48
maximal N O 2
4.5FeVTW S-550
46
4.5FeVTW S-600 4.5FeVTW S-650 4.5FeVTW S-700
30
N2O / ppm
VTW S-650
N O at 10 ppm NH 2
20
3
slip
4.5FeVTW S-550 4.5FeVTW S-600 4.5FeVTW S-650
10
4.5FeVTW S-700 VTW S-650
0 200
250
300
350
400
450
500
550
Temperature / °C
Figure S3: a) N2 O production of 4.5FeVTWS calcined at 550 , 600 , 650 and 700 for 10 h. Reaction conditions: 0 - 600 ppm NH3 , 500 ppm NO, 10 vol% O2 , 5 vol% H2 O (bal. N2 ), GHSV: 50 000 h−1 .
S4
