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Journal of Hazardous Materials
journal homepage: www.elsevier.com/locate/jhazmat
Irregular influence of alkali metals on Cu-SAPO-34 catalyst for selective
catalytic reduction of NO
x
with ammonia
Guangpeng Yang
a,b
, Xuesen Du
a,
*, Jingyu Ran
a,
*, Xiangmin Wang
a
, Yanrong Chen
a
, Li Zhang
a
,
Vladislav Rac
c
, Vesna Rakic
c
, John Crittenden
b
a
Key Laboratory of Low-Grade Energy Utilization Technologies and Systems, School of Energy and Power Engineering, Chongqing University, Chongqing, 400044, China
b
Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, United States
c
Faculty of Agriculture, Department of Chemistry, University of Belgrade, Nemanjina 6, 11080, Zemun, Serbia
GRAPHICAL ABSTRACT
ARTICLE INFO
Editor: Xiaohong Guan
Keywords:
Cu-SAPO-34
Alkali metal
Migration
Cu species
ABSTRACT
SCR activity of Cu-SAPO-34 catalyst was reduced by alkali metal ions. The alkali metals ions (Li
+
, Na
+
and K
+
)
have shown irregular influences on Cu-SAPO-34. The order of poisoning strengths under 400 °C was found to be:
Na
+
>K
+
> Li
+
, which is not consistent with the basicities of their corresponding metals. Experimental re-
sults and calculations showed that the alkali metal ions readily replace H
+
and Cu
2+
/Cu
+
ions. These exchanges
result in the loss of Brønsted acid sites and migration of isolated Cu
2+
ions in Cu-SAPO-34, which decrease the
NH
3
-SCR activity. Both the basicity and ion diameter will affect the exchanging behavior of an alkali ion. Na
+
and Li
+
ions will influence both H
+
and Cu
2+
/Cu
+
ions but K
+
ions only preferably replace the H
+
. We
hypothesize that K
+
cannot enter into a small ring (6-membered ring) to replace a Cu
2+
/Cu
+
ion because of its
large ion diameter. The displaced Cu
2+
/Cu
+
ions will transfer to adjacent unbonded Al site to form a CuAlO
2
species.
1. Introduction
The selective catalytic reduction of NO
x
with NH
3
(NH
3
-SCR) is an
effective way to reduce the NO
x
emission from both mobile and point
sources. The Cu-SAPO-34 catalyst used for removing NO
x
in mobile
sources has drawn much attention, because of its high destruction ef-
ficiency for NO
x
reduction over a wide temperature range and superior
resistance to hydrothermal aging, compared with traditional V-based
https://doi.org/10.1016/j.jhazmat.2019.122007
Received 24 September 2019; Received in revised form 7 December 2019; Accepted 30 December 2019
⁎
Corresponding authors.
E-mail addresses: gpyang@cqu.edu.cn (G. Yang), xuesendu@cqu.edu.cn (X. Du), ranjy@cqu.edu.cn (J. Ran).
Journal of Hazardous Materials 387 (2020) 122007
Available online 31 December 2019
0304-3894/ © 2019 Elsevier B.V. All rights reserved.
T