Fully copper-exchanged high-silica LTA zeolites as unrivaled hydrothermally stable NH3-SCR catalysts

Taekyung Ryu; Nak Ho Ahn; Seungwan Seo; Jung Cho; Hyojun Kim; Donghui Jo; Gi Tae Park; Pyung Soon Kim; Chang Hwan Kim; Elliott L. Bruce; Paul A. Wright; In-Sik Nam; Suk Bong Hong

doi:10.1002/anie.201610547

Fully copper-exchanged high-silica LTA zeolites as unrivaled hydrothermally stable NH₃-SCR catalysts

Taekyung Ryu, Nak Ho Ahn, Seungwan Seo, Jung Cho, Hyojun Kim, Donghui Jo, Gi Tae Park, Pyung Soon Kim, Chang Hwan Kim, Elliott L. Bruce, Paul A. Wright, In-Sik Nam, Suk Bong Hong

Research output: Contribution to journal › Article › peer-review

Abstract

Diesel engine technology is still the most effective solution to meet tighter CO₂regulations in the mobility and transport sector. In implementation of fuel-efficient diesel engines, the poor thermal durability of lean nitrogen oxides (NO_x) aftertreatment systems remains as one major technical hurdle. Divalent copper ions when fully exchanged into high-silica LTA zeolites are demonstrated to exhibit excellent activity maintenance for NO_x reduction with NH₃ under vehicle simulated conditions even after hydrothermal aging at 900 °C, a critical temperature that the current commercial Cu-SSZ-13 catalyst cannot overcome owing to thermal deactivation. Detailed structural characterizations confirm the presence of Cu²⁺ ions only at the center of single 6-rings that act not only as a catalytically active center, but also as a dealumination suppressor. The overall results render the copper-exchanged LTA zeolite attractive as a viable substitute for Cu-SSZ-13.

Original language	English
Pages (from-to)	3256-3260
Number of pages	5
Journal	Angewandte Chemie International Edition
Volume	56
Issue number	12
Early online date	18 Jan 2017
DOIs	https://doi.org/10.1002/anie.201610547
Publication status	Published - 13 Mar 2017

Keywords

Cu-LTA
Heterogeneous catalysis
Hydrothermal stability
Selective catalytic reduction
Zeolites

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10.1002/anie.201610547

Wright_2016_ACIE_LTAZeolites_AAM
© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at: https://doi.org/10.1002/anie.201610547
Accepted author manuscript, 1.08 MB
SuppInfo_Wright_ACIE_LTAZeolites
© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. This work has been made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at: https://doi.org/10.1002/anie.201610547
Accepted author manuscript, 1.55 MB

Cite this

@article{c722e4ba2e9e4659b2b11f4a568274a8,

title = "Fully copper-exchanged high-silica LTA zeolites as unrivaled hydrothermally stable NH3-SCR catalysts",

abstract = "Diesel engine technology is still the most effective solution to meet tighter CO2 regulations in the mobility and transport sector. In implementation of fuel-efficient diesel engines, the poor thermal durability of lean nitrogen oxides (NOx) aftertreatment systems remains as one major technical hurdle. Divalent copper ions when fully exchanged into high-silica LTA zeolites are demonstrated to exhibit excellent activity maintenance for NOx reduction with NH3 under vehicle simulated conditions even after hydrothermal aging at 900 °C, a critical temperature that the current commercial Cu-SSZ-13 catalyst cannot overcome owing to thermal deactivation. Detailed structural characterizations confirm the presence of Cu2+ ions only at the center of single 6-rings that act not only as a catalytically active center, but also as a dealumination suppressor. The overall results render the copper-exchanged LTA zeolite attractive as a viable substitute for Cu-SSZ-13.",

keywords = "Cu-LTA, Heterogeneous catalysis, Hydrothermal stability, Selective catalytic reduction, Zeolites",

author = "Taekyung Ryu and Ahn, \{Nak Ho\} and Seungwan Seo and Jung Cho and Hyojun Kim and Donghui Jo and Park, \{Gi Tae\} and Kim, \{Pyung Soon\} and Kim, \{Chang Hwan\} and Bruce, \{Elliott L.\} and Wright, \{Paul A.\} and In-Sik Nam and Hong, \{Suk Bong\}",

note = "We acknowledge financial support from the National Creative Research Initiative Program (2012R1A3A2048833) through the National Research Foundation of Korea and from Hyundai Motor Group. We also thank J. Y. Koo (POSTECH) for assistance with ESR measurements, K.-S. Lee and Y. H. Jung (8C and 9B, PAL, respectively) for help in X-ray absorption and diffraction data, S. P. Thompson (I11,DLS) for help in obtaining powder X-ray diffraction data, and PAL and DLS for beam time. PAL is supported by MSIP and POSTECH. We acknowledge financial support from the National Creative Research Initiative Program (2012R1A3A2048833) through the National Research Foundation of Korea and from Hyundai Motor Group. We also thank J. Y. Koo (POSTECH) for assistance with ESR measurements, K.-S. Lee and Y. H. Jung (8C and 9B, PAL, respectively) for help in X-ray absorption and diffraction data, S. P. Thompson (I11,DLS) for help in obtaining powder X-ray diffraction data, and PAL and DLS for beam time. PAL is supported by MSIP and POSTECH.",

year = "2017",

month = mar,

day = "13",

doi = "10.1002/anie.201610547",

language = "English",

volume = "56",

pages = "3256--3260",

journal = "Angewandte Chemie International Edition",

issn = "1521-3773",

publisher = "John Wiley \& Sons, Ltd",

number = "12",

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TY - JOUR

T1 - Fully copper-exchanged high-silica LTA zeolites as unrivaled hydrothermally stable NH3-SCR catalysts

AU - Ryu, Taekyung

AU - Ahn, Nak Ho

AU - Seo, Seungwan

AU - Cho, Jung

AU - Kim, Hyojun

AU - Jo, Donghui

AU - Park, Gi Tae

AU - Kim, Pyung Soon

AU - Kim, Chang Hwan

AU - Bruce, Elliott L.

AU - Wright, Paul A.

AU - Nam, In-Sik

AU - Hong, Suk Bong

N1 - We acknowledge financial support from the National Creative Research Initiative Program (2012R1A3A2048833) through the National Research Foundation of Korea and from Hyundai Motor Group. We also thank J. Y. Koo (POSTECH) for assistance with ESR measurements, K.-S. Lee and Y. H. Jung (8C and 9B, PAL, respectively) for help in X-ray absorption and diffraction data, S. P. Thompson (I11,DLS) for help in obtaining powder X-ray diffraction data, and PAL and DLS for beam time. PAL is supported by MSIP and POSTECH. We acknowledge financial support from the National Creative Research Initiative Program (2012R1A3A2048833) through the National Research Foundation of Korea and from Hyundai Motor Group. We also thank J. Y. Koo (POSTECH) for assistance with ESR measurements, K.-S. Lee and Y. H. Jung (8C and 9B, PAL, respectively) for help in X-ray absorption and diffraction data, S. P. Thompson (I11,DLS) for help in obtaining powder X-ray diffraction data, and PAL and DLS for beam time. PAL is supported by MSIP and POSTECH.

PY - 2017/3/13

Y1 - 2017/3/13

N2 - Diesel engine technology is still the most effective solution to meet tighter CO2 regulations in the mobility and transport sector. In implementation of fuel-efficient diesel engines, the poor thermal durability of lean nitrogen oxides (NOx) aftertreatment systems remains as one major technical hurdle. Divalent copper ions when fully exchanged into high-silica LTA zeolites are demonstrated to exhibit excellent activity maintenance for NOx reduction with NH3 under vehicle simulated conditions even after hydrothermal aging at 900 °C, a critical temperature that the current commercial Cu-SSZ-13 catalyst cannot overcome owing to thermal deactivation. Detailed structural characterizations confirm the presence of Cu2+ ions only at the center of single 6-rings that act not only as a catalytically active center, but also as a dealumination suppressor. The overall results render the copper-exchanged LTA zeolite attractive as a viable substitute for Cu-SSZ-13.

AB - Diesel engine technology is still the most effective solution to meet tighter CO2 regulations in the mobility and transport sector. In implementation of fuel-efficient diesel engines, the poor thermal durability of lean nitrogen oxides (NOx) aftertreatment systems remains as one major technical hurdle. Divalent copper ions when fully exchanged into high-silica LTA zeolites are demonstrated to exhibit excellent activity maintenance for NOx reduction with NH3 under vehicle simulated conditions even after hydrothermal aging at 900 °C, a critical temperature that the current commercial Cu-SSZ-13 catalyst cannot overcome owing to thermal deactivation. Detailed structural characterizations confirm the presence of Cu2+ ions only at the center of single 6-rings that act not only as a catalytically active center, but also as a dealumination suppressor. The overall results render the copper-exchanged LTA zeolite attractive as a viable substitute for Cu-SSZ-13.

KW - Cu-LTA

KW - Heterogeneous catalysis

KW - Hydrothermal stability

KW - Selective catalytic reduction

KW - Zeolites

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UR - https://www.scopus.com/pages/publications/85009758496

U2 - 10.1002/anie.201610547

DO - 10.1002/anie.201610547

M3 - Article

SN - 1521-3773

VL - 56

SP - 3256

EP - 3260

JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

IS - 12

ER -

Fully copper-exchanged high-silica LTA zeolites as unrivaled hydrothermally stable NH₃-SCR catalysts

Abstract

Keywords

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