Experimental Setup

Fixed-bed quartz tube

reactor:

h = 20 cm

d = 0.6 cm

mCat = 0.2 g

Reaction Conditions:

GHSV = 30,000 h-1

c(NO) = 500 ppm

c(NH3) = 575 ppm

= 120 mL min-1

c(O2) = 4 Vol.-%

Selective catalytic reduction of NOx by NH3 (NH3-SCR) is

used as an efficient technology to eliminate NOx from the

diesel exhausts. Several research groups have reported

property-activity relationships for Cu-containing molecular

sieves, e.g., Cu-ZSM-5 [1] or Cu-SSZ-13 [2]. Additionally,

mesopores have been shown to provide high dispersion of

the metal component in comparison to conventional

microporous materials and thus also enhanced activity and

N2 selectivity in NH3-SCR. However, the catalytic

properties of Cu-Y has been less extensively investigated

compared to other Cu-containing zeolites [3]. In view of

these challenges, zeolite Y was synthesized and exposed to

a variety of acid or base treatments [4]. In this study, the

effect of the structural and textural properties of the zeolites

on the nature and distribution of copper species and the

associated catalytic properties were investigated over

hierarchical micro-/mesoporous Cu-Y.

Result and Discussion

NH3-SCR over Copper-exchanged Zeolite Y

R. S. R. Suharbiansaha, K. Góra-Marekb, K. Pyrab, R. Gläsera, M. JabłońskaaaInstitute of Chemical Technology, Universität Leipzig, Linnestr. 3, 04103, Leipzig, Germany

bFaculty of Chemistry, Jagiellonian University in Krakow, Gronostajowa 2, 30-387 Krakow, Poland

M. Sc. Rujito Sesariojiwandono

Ridho S.

Institute of Chemical Technology

Linnéstr. 3 | 04103 Leipzig

+49 341 97 36318

rujito.suharbiansah@uni-leipzig.de

Introduction

References

Institute of Chemical Technology

Contact

Conclusions Across the investigated materials, copper species were mainly

present as isolated cations (the light blue colored ion-exchanged

materials) and bulky CuO clusters Cu-Y (Na2H2EDTA)

The Cu2+ species serve as active sites for NH3-SCR, while NH3

is oxidized to NO over CuO sites

CuY Cu-Y (DEA)

Cu-Y (EDTA)

Cu-Y (NaOH)

0

2

4

6

8

10

Na c

onte

nt

/ w

t.-%

Cu c

onte

nt

/ w

t.-%

0

2

4

6

8

10

Copper particles are

dispersed

homogenously

throughout the

zeolite samples

Cu-Y

30 µm

2 µm

Experimental Section

ሶV

4NO + 4NH3 + O2 4N2 + 6H2O

2NO2 + 4NH3 + O2 3N2 + 6H2O

Catalytic Investigations

Selective Catalytic Reduction

[1] J. Zhao, G. Wang, L. Qin, H. Li, Y. Chen, B. Liu,

Catal. Commun. 73 (2016) 98-102.

[2] S. Shrestha, M.P. Harold, K. Kamasamudram, A.

Kumar, L. Olsson, K. Leistner, Catal. Today 267

(2016) 130-144.

[3] A.A. Dabbawala, V. Tzitzios, K. Sunny, K.

Polychronopoulou, G. Basina, I. Ismail, V. Pillai, A.

Tharalekshmy, S. Stephen, S.M. Alhassan, Surf. Coat.

Technol. 350 (2018) 369-375.

[4] M. Rutkowska, I. Pacia, S. Basąg, A. Kowalczyk, Z.

Piwowarska, M. Duda, K.A. Tarach, K. Góra-Marek,

M. Michalik, U. Díaz, L. Chmielarz, Microporous

Mesoporous Mater. 246 (2017) 193-206.

Acknowledgements:

100 150 200 250 300 350 400 450

0

5

10

15

20

25

30

35

Cu-Y

Cu-Y (DEA)

Cu-Y (Na2H2EDTA)

Cu-Y (NaOH)

Cu-Y (TPAOH)

N2O

yie

ld /

%

Temperature / oC

200 300 400 500 600 700 800 900

Cu+/Cu2+ CT

Kubelk

a-M

unk function /

arb

.u.

Wavelength / cm-1

Cu-Y

Cu-Y (DEA)

Cu-Y (Na2H2EDTA)

Cu-Y (NaOH)

Cu-Y (TPAOH)

Cu2+ d-d

Charge transfer (CT)

from framework

oxygen to isolated Cu+

and/or Cu2+

2200 2150 2100 2050

Absorb

ance /

arb

.u.

Wavenumber / cm-1

21302142

Cu+oxo(CO)Cu+

exch(CO)

2155

2179Cu+exch(CO)2

2151Cu-Y

Cu-Y (DEA)

Cu-Y (Na2H2EDTA)

Cu-Y (NaOH)

Cu-Y (TPAOH)

CO sorption revealed

monocarbonyls and

dicarbonyls of Cu+ in the

exchange positions

(Cu+exch(CO), Cu+

exch(CO)2)

and monocarbonyls of Cu+

oxo-species (Cu+oxo(CO).

d-d transition - presence

of aggregated CuOx

The N2O yield does not

vary significantly within

the tested catalysts and

does not exceed more

than 30% in the studied

temperature range of 100-

450 ̊C

Catalytic tests

SCR CatalystZeolite Y

• Catalyst morphology

50 100 150 200 250 300 350 400 450 500

20

40

60

80

100

NO

convers

ion /

%

Temperature / oC

Cu-Y

Cu-Y (DEA)

Cu-Y (Na2H2EDTA)

Cu-Y (NaOH)

Cu-Y (TPAOH)• Copper species in

catalysts

• Catalyst composition

Treatment with:

• DEA – diethylamine; NaOH – sodium hydroxide

• Na2H2EDTA – disodium ethylenediamine tetraacetate

• TPAOH – tetrapropylammonium hydroxide

Cu-Y (DEA)Cu-Y (NaOH)Cu-Y (Na2H2EDTA)

Cu-Y (TPAOH)