Supplementary information for “Ceria based diesel soot oxidation catalysts prepared by
flame spray pyrolysis”
Jakob M. Christensen1, Jan-Dierk Grunwaldt1,2 and Anker D. Jensen1*
1
Department of Chemical and Biochemical Engineering, Technical University of Denmark, Søltofts
Plads Building 229, 2800 Kgs. Lyngby (Denmark)
2
Institute for Technical and Polymer Chemistry, Karlsruhe Institute of Technology, Engesserstrasse
20, 76131 Karlsruhe (Germany)
*aj@kt.dtu.dk
700
650
o
Tmax [ C]
600
550
500
450
400
350
0
1
2
3
4
5
6
7
8
9
10
Crushing time [min]
Figure S1 The temperature of maximal oxidation rate (Tmax) for a mixture of flame made CeO2 and NIST SRM
2975 soot as a function of the time the mixture is crushed together in an agate mortar. The figure illustrates that
there is little additional gain by increasing the crushing time beyond 5-6 minutes. Experimental conditions:
Soot/catalyst 1/5 wt/wt, 100 NmL/min, 10 vol% O2 in N2.
Figure S2 TEM image of the flame made ceria sample.
Figure S3 TEM image of the flame made ceria sample.
Figure S4 TEM image of the flame made ceria sample.
Figure S5 TEM image of the flame made ceria sample.
Table S1 Comparison of reported temperatures of maximal oxidation rate (with O2 as the oxidant)
for CeO2 catalyzed soot oxidation with tight soot/catalyst contact.
Study
This work - NIST soot
This work – S-A carbon c)
Machida et al. 2008
This work - NIST soot d)
This work - FSP soot e)
Saab et al. 2007
Shimizu et al. 2010
Ikeue et al. 2009
Aouad et al. 2009
Issa et al. 2009
Kockrick et al. 2008
Soutward & Basso 2008 g)
Zhang et al. 2010
Hansen et al. 2013
Bokova et al. 2005
Li et al. 2011
Aneggi et al. 2007
Lim et al. 2011
Yamazaki et al. 2011
van Doorn et al. 1992
Hensgen & Stöwe 2011
Muroyama et al. 2010
Palmisano et al. 2006
Neeft et al. 1996
Oliveira et al. 2012
Fang et al. 2008
Wu et al. 2007
Bueno-Lopez et al. 2005
a)
b)
Ramping
Tmax, cat O2 conc. Soot/Catalyst Tmax, soot T a) Sg
2
rate
Ref.
[m
/g]
[wt/wt]
[°C] [vol%]
[°C] [°C]
[°C/min]
382
10
1/5
667
-285 182
10
433
10
1/5
718
-285 182
10
393
10
1/20
668
-275
45
10
[1]
393
10
1/5
667
-274 149
10
336
10
1/5
608
-272 182
10
360
21
1/19
632
-272
83
5
[2]
360
20
1/80
630
-270 115
5
[3]
397
10
1/20
660
-263 157
10
[4]
384
21
1/9
629
-245
93
5
[5]
425
10
1/19
670
-245 120
10
[6]
f)
414
6
1/20
640
-226 82
5
[7]
376
21
600
-224
10
[8]
380
10
1/9
603
-223 50.6
5
[9]
61
10
[10]
442
10
1/5
662
-220
389
21
1/5
609
-220
53
5
[11]
397
10
1/9
600
-200 50.6
5
[12]
385
21
1/20
585
-200
57
10
[13]
h)
63
10
[14]
448
21
~1/19
648
-200
462
10
1/19
660
-198 77.8
20
[15]
410
15
1/4
600
-190
5
5
[16]
407 i)
8
1/4
593
-186
60
2
[17]
555
21
1/4
725
-170 27.3
5
[18]
405
21
1/9
560
-155
60
5
[19]
567
21
1/2
717
-150
10
[20]
474
21
1/20
622
-148 30.3
10
[21]
485
21
1/9
594
-109 17.5
10
[22]
505
10
1/10
600
-95
6
10
[23]
575
21
1/4
613
-38
3
10
[24]
Tmax,cat-Tmax, soot.
Specific surface area of the catalyst.
c)
The carbonaceous material is carbon nanopowder from Sigma-Aldrich
d)
Catalyst calcined 2 h at 500 °C before use.
e)
Catalytic oxidation of soot produced with the FSP setup. See also the soot characterization results in table S2.
f)
Estimated from the crystallite size of 9.6 nm.
g)
This sample contains 33 % Ce and 77 % Zr. The T max value for pure soot is estimated from the value obtained with a
Pt-CeO2-Al2O3 catalyst, which is reported by Soutward and Basso not to yield any improvement compared to noncatalytic soot oxidation.
h)
Tmax,soot is the value given by Lim et al. for soot in loose contact with TiO 2.
i)
Temperature corresponding to 50% conversion.
b)
Table S2 Properties of the 3 investigated soot samples
C [wt%]
H [wt%]
Surface area [m2/g]
Tmax [°C]
NIST SRM 2975 a)
87.17
1.53
91 b)
667
FSP soot
93.25
2.88
89
608
Sigma Aldrich Nanocarbon
99.64
0.30
213
718
a) As the only one of the 3 samples NIST SRM 2975 also exhibits signs of smaller amounts of organically bound sulfur
and nitrogen (see also Im et al.[25]), but the presently used standards and methods did not allow an accurate
quantification of the contents of S and N.
b)
The measured surface area of SRM 2975 is in good agreement with the calibration certificate from NIST (which also
reports 91 m2/g).
References
[1] Machida M, Murata Y, Kishikawa K, Zhang D, Ikeue K (2008) Chem Mater 20:4489-4494.
[2] Saab E, Aouad S, Abi-Aad E, Bokova M, Zhilinskaya E, Aboukaïs A (2007) Kin Catal 48:841846.
[3] Shimizu K, Kawachi H, Satsuma A (2010) Appl Catal B 96:169-175.
[4] Ikeue K, Kobayashi S, Machida M (2009) J Ceram Soc Jap 117:1153-1157.
[5] Aouad S, Abi-Aad E, Aboukais A (2009) Appl Catal B 88:249-256.
[6] Issa M, Mahzoul H, Brillard A, Brilhac JF (2009) Chem Eng Technol 32:1859-1865.
[7] Kockrick E, Schrage C, Grigas A, Geiger D, Kaskel S (2008) J Solid State Chem 181:16141620.
[8] Southward BWL, Basso S (2008) SAE paper 2008-01-0481.
[9] Zhang Z, Han D, Wei S, Zhang Y (2010) J Catal 276:16-23.
[10] Hansen BB, Jensen AD, Jensen PA (2013) Fuel 106:234-240.
[11] Bokova M, Decarne C, Abi-Aad E, Pryakhin A, Lunin V, Aboukais A (2005) Thermochim
Acta 428:165-171.
[12] Li X, Wei S, Zhang Z, Zhang Y, Wang Z, Su Q, Gao X (2011) Catal Today 175:112-116.
[13] Aneggi E, de Leitenburg C, Dolcetti G, Trovarelli A (2007) Top Catal 42:319-322.
[14] Lim C-B, Kusaba H, Einaga H, Teraoka Y (2011) Catal Today 175:106-111.
[15] Yamazaki K, Kayama T, Dong F, Shinjoh H (2011) J Catal 282:289-298.
[16] Van Doorn J, Varloud J, Meriaudeau P, Perrichon V, Chevrier M, Gauthier C (1992) Appl
Catal B 1:117-127.
[17] Hensgen L, Stöwe K (2011) Catal Today 159:100-107.
[18] Muroyama H, Hano S, Matsui T, Eguchi K (2010) Catal Today 153:133-135.
[19] Palmisano P, Russo N, Fino P, Fino D, Badini C (2006) Appl Catal B 69:85-92.
[20] Neeft J, Makkee M, Moulijn JA (1996) Chem Eng J 64:295-302.
[21] Oliveira CF, Garcia FAC, Araújo DR, Macedo JL, Dias SCL, Dias JA (2012) Appl Catal A
413-141:292-300.
[22] Fang P, Luo MF, Lu JQ, Cen SQ, Yan XY, Wang XX (2008) Thermochim Acta 478:45-50.
[23] Wu X, Liu D, Li K, Li J, Weng D (2007) Catal Commun 8:1274-1278.
[24] Bueno-Lopez A, Krishna K, Makkee M, Moulijn J (2005) J Catal 230:237-248.
[25] Im J, Lee CM, Coates JT (2008) Chemosphere 71:621-628.