Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers

Khivantsev, Konstantin; Jaegers, Nicholas R.; Kovarik, Libor; Hanson, Jonathan C.; Tao, Franklin (Feng); Tang, Yu; Zhang, Xiaoyan; Koleva, Iskra Z.; Aleksandrov, Hristiyan A.; Vayssilov, Georgi N.; Wang, Yong; Gao, Feng; Szanyi, János

doi:10.1002/anie.201809343

Title: Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO _x Adsorbers

Abstract

Abstract The majority of harmful atmospheric CO and NO _x emissions are from vehicle exhausts. Although there has been success addressing NO _x emissions at temperatures above 250 °C with selective catalytic reduction technology, emissions during vehicle cold start (when the temperature is below 150 °C), are a major challenge. Herein, we show we can completely eliminate both CO and NO _x emissions simultaneously under realistic exhaust flow, using a highly loaded (2 wt %) atomically dispersed palladium in the extra‐framework positions of the small‐pore chabazite material as a CO and passive NO _x adsorber. Until now, atomically dispersed highly loaded (>0.3 wt %) transition‐metal/SSZ‐13 materials have not been known. We devised a general, simple, and scalable route to prepare such materials for Pt ^II and Pd ^II . Through spectroscopy and materials testing we show that both CO and NO _x can be simultaneously completely abated with 100 % efficiency by the formation of mixed carbonyl‐nitrosyl palladium complex in chabazite micropore.

Authors:

^[1]; Jaegers, Nicholas R. ^[2]; Kovarik, Libor ^[1]; Hanson, Jonathan C. ^[3]; Tao, Franklin ^[4]; Tang, Yu ^[5]; Zhang, Xiaoyan ^[5]; Koleva, Iskra Z. ^[6]; Aleksandrov, Hristiyan A. ^[6]; Vayssilov, Georgi N. ^[6]; Wang, Yong ^[2]; Gao, Feng ^[1];

^[1]

Institute for Integrated Catalysis Pacific Northwest National Laboratory Richland WA 99352 USA
Institute for Integrated Catalysis Pacific Northwest National Laboratory Richland WA 99352 USA, Voiland School of Chemical Engineering and Bioengineering Washington State University Pullman WA 99163 USA
Chemistry Department Brookhaven National Laboratory Uptown NY 11973 USA
(Feng) [Department of Chemical and Petroleum Engineering and Center for Environmentally Beneficial Catalysis University of Kansas Lawrence KS 66045 USA
Department of Chemical and Petroleum Engineering and Center for Environmentally Beneficial Catalysis University of Kansas Lawrence KS 66045 USA
Faculty of Chemistry and Pharmacy University of Sofia 1126 Sofia Bulgaria

Publication Date:: Mon Nov 12 00:00:00 EST 2018

Sponsoring Org.:: USDOE

OSTI Identifier:: 1481809

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition) Journal Volume: 57 Journal Issue: 51; Journal ID: ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Khivantsev, Konstantin, Jaegers, Nicholas R., Kovarik, Libor, Hanson, Jonathan C., Tao, Franklin, Tang, Yu, Zhang, Xiaoyan, Koleva, Iskra Z., Aleksandrov, Hristiyan A., Vayssilov, Georgi N., Wang, Yong, Gao, Feng, and Szanyi, János. Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers.  Germany: N. p., 2018. 
Web.  doi:10.1002/anie.201809343.

Copy to clipboard


                    Khivantsev, Konstantin, Jaegers, Nicholas R., Kovarik, Libor, Hanson, Jonathan C., Tao, Franklin, Tang, Yu, Zhang, Xiaoyan, Koleva, Iskra Z., Aleksandrov, Hristiyan A., Vayssilov, Georgi N., Wang, Yong, Gao, Feng, & Szanyi, János. Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers.  Germany.  https://doi.org/10.1002/anie.201809343

Copy to clipboard


                    Khivantsev, Konstantin, Jaegers, Nicholas R., Kovarik, Libor, Hanson, Jonathan C., Tao, Franklin, Tang, Yu, Zhang, Xiaoyan, Koleva, Iskra Z., Aleksandrov, Hristiyan A., Vayssilov, Georgi N., Wang, Yong, Gao, Feng, and Szanyi, János. Mon .  
"Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers".  Germany.  https://doi.org/10.1002/anie.201809343.

Copy to clipboard


                    
@article{osti_1481809,

  title        = {Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers},

  author       = {Khivantsev, Konstantin and Jaegers, Nicholas R. and Kovarik, Libor and Hanson, Jonathan C. and Tao, Franklin and Tang, Yu and Zhang, Xiaoyan and Koleva, Iskra Z. and Aleksandrov, Hristiyan A. and Vayssilov, Georgi N. and Wang, Yong and Gao, Feng and Szanyi, János},

  abstractNote = {Abstract The majority of harmful atmospheric CO and NO x emissions are from vehicle exhausts. Although there has been success addressing NO x emissions at temperatures above 250 °C with selective catalytic reduction technology, emissions during vehicle cold start (when the temperature is below 150 °C), are a major challenge. Herein, we show we can completely eliminate both CO and NO x emissions simultaneously under realistic exhaust flow, using a highly loaded (2 wt %) atomically dispersed palladium in the extra‐framework positions of the small‐pore chabazite material as a CO and passive NO x adsorber. Until now, atomically dispersed highly loaded (>0.3 wt %) transition‐metal/SSZ‐13 materials have not been known. We devised a general, simple, and scalable route to prepare such materials for Pt II and Pd II . Through spectroscopy and materials testing we show that both CO and NO x can be simultaneously completely abated with 100 % efficiency by the formation of mixed carbonyl‐nitrosyl palladium complex in chabazite micropore.},

  doi          = {10.1002/anie.201809343},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 51,

  volume       = 57,

  place        = {Germany},

  year         = {Mon Nov 12 00:00:00 EST 2018},

  month        = {Mon Nov 12 00:00:00 EST 2018}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (Publisher)

Publisher's Version of Record
https://doi.org/10.1002/anie.201809343

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 113 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Selective Catalytic Reduction over Cu/SSZ-13: Linking Homo- and Heterogeneous Catalysis
journal, March 2017

Gao, Feng; Mei, Donghai; Wang, Yilin
Journal of the American Chemical Society, Vol. 139, Issue 13
DOI: 10.1021/jacs.7b01128

Polycarbonyl species in Pt/H–ZSM-5: FTIR spectroscopic study of 12CO–13CO co-adsorption
journal, July 2005

Chakarova, Kristina; Mihaylov, Mihail; Hadjiivanov, Konstantin
Catalysis Communications, Vol. 6, Issue 7
DOI: 10.1016/j.catcom.2005.04.007

Co-ordination chemistry of palladium cations in Pd-H-ZSM-5 as revealed by FTIR spectra of adsorbed and co-adsorbed probe molecules (CO and NO)
journal, January 2004

Chakarova, K.; Ivanova, E.; Hadjiivanov, K.
Phys. Chem. Chem. Phys., Vol. 006, Issue 13
DOI: 10.1039/B401934B

A Common Intermediate for N ₂ Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes
journal, August 2013

Kwak, Ja Hun; Lee, Jong H.; Burton, Sarah D.
Angewandte Chemie International Edition, Vol. 52, Issue 38
DOI: 10.1002/anie.201303498

Shape selective and hydrogen spillover approach in the design of sulfur-tolerant hydrogenation catalysts
journal, October 2006

Yang, H.; Chen, H.; Chen, J.
Journal of Catalysis, Vol. 243, Issue 1
DOI: 10.1016/j.jcat.2006.06.026

Advances in Automobile Emissions Control Catalysis
journal, June 2016

Wang, Di; Epling, Bill; Nova, Isabella
Catalysis Today, Vol. 267
DOI: 10.1016/j.cattod.2016.04.001

Catalytic decomposition of ammonia in a membrane reactor
journal, December 1994

Collins, John P.; Way, J. Douglas
Journal of Membrane Science, Vol. 96, Issue 3
DOI: 10.1016/0376-7388(94)00138-3

Coordinatively Unsaturated Al3+ Centers as Binding Sites for Active Catalyst Phases of Platinum on -Al2O3
journal, September 2009

Kwak, J. H.; Hu, J.; Mei, D.
Science, Vol. 325, Issue 5948
DOI: 10.1126/science.1176745

Low-Temperature Transformation of Methane to Methanol on Pd ₁ O ₄ Single Sites Anchored on the Internal Surface of Microporous Silicate
journal, September 2016

Huang, Weixin; Zhang, Shiran; Tang, Yu
Angewandte Chemie, Vol. 128, Issue 43
DOI: 10.1002/ange.201604708

Low Temperature NO Storage of Zeolite Supported Pd for Low Temperature Diesel Engine Emission Control
journal, June 2016

Chen, Hai-Ying; Collier, Jillian E.; Liu, Dongxia
Catalysis Letters, Vol. 146, Issue 9
DOI: 10.1007/s10562-016-1794-6

Al2O3-based passive NOx adsorbers for low temperature applications
journal, July 2015

Ji, Yaying; Bai, Shuli; Crocker, Mark
Applied Catalysis B: Environmental, Vol. 170-171
DOI: 10.1016/j.apcatb.2015.01.025

Coordination and Organometallic Chemistry of Metal−NO Complexes
journal, April 2002

Hayton, Trevor W.; Legzdins, Peter; Sharp, W. Brett
Chemical Reviews, Vol. 102, Issue 4
DOI: 10.1021/cr000074t

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity
journal, May 2007

Zhan, Bi-Zeng; Iglesia, Enrique
Angewandte Chemie International Edition, Vol. 46, Issue 20
DOI: 10.1002/anie.200700128

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species
journal, December 2009

Rivallan, Mickaël; Seguin, Etienne; Thomas, Sébastien
Angewandte Chemie International Edition, Vol. 49, Issue 4
DOI: 10.1002/anie.200905181

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol
journal, June 2018

Sushkevich, Vitaly L.; Palagin, Dennis; van Bokhoven, Jeroen A.
Angewandte Chemie International Edition, Vol. 57, Issue 29
DOI: 10.1002/anie.201802922

Activation of Pd/SSZ-13 catalyst by hydrothermal aging treatment in passive NO adsorption performance at low temperature for cold start application
journal, September 2017

Ryou, YoungSeok; Lee, Jaeha; Cho, Sung June
Applied Catalysis B: Environmental, Vol. 212
DOI: 10.1016/j.apcatb.2017.04.077

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species
journal, December 2009

Rivallan, Mickaël; Seguin, Etienne; Thomas, Sébastien
Angewandte Chemie, Vol. 122, Issue 4
DOI: 10.1002/ange.200905181

On the hydrothermal stability of Cu/SSZ-13 SCR catalysts
journal, June 2018

Gao, Feng; Szanyi, János
Applied Catalysis A: General, Vol. 560
DOI: 10.1016/j.apcata.2018.04.040

Molecular Level Understanding of How Oxygen and Carbon Monoxide Improve NO _x Storage in Palladium/SSZ-13 Passive NO _x Adsorbers: The Role of NO ⁺ and Pd(II)(CO)(NO) Species
journal, April 2018

Khivantsev, Konstantin; Gao, Feng; Kovarik, Libor
The Journal of Physical Chemistry C, Vol. 122, Issue 20
DOI: 10.1021/acs.jpcc.8b01007

Mercaptosilane-Assisted Synthesis of Metal Clusters within Zeolites and Catalytic Consequences of Encapsulation
journal, July 2010

Choi, Minkee; Wu, Zhijie; Iglesia, Enrique
Journal of the American Chemical Society, Vol. 132, Issue 26
DOI: 10.1021/ja102778e

Effects of CO on Pd/BEA Passive NOx Adsorbers
journal, January 2017

Vu, Anh; Luo, Jinyong; Li, Junhui
Catalysis Letters, Vol. 147, Issue 3
DOI: 10.1007/s10562-017-1976-x

The Adsorption of NO and Reaction of NO with O2on H-, NaH-, CuH-, and Cu-ZSM-5: Anin SituFTIR Investigation
journal, November 1996

Szanyi, János; Paffett, Mark T.
Journal of Catalysis, Vol. 164, Issue 1
DOI: 10.1006/jcat.1996.0378

Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
journal, September 2015

Ding, K.; Gulec, A.; Johnson, A. M.
Science, Vol. 350, Issue 6257
DOI: 10.1126/science.aac6368

Low-Temperature Transformation of Methane to Methanol on Pd ₁ O ₄ Single Sites Anchored on the Internal Surface of Microporous Silicate
journal, September 2016

Huang, Weixin; Zhang, Shiran; Tang, Yu
Angewandte Chemie International Edition, Vol. 55, Issue 43
DOI: 10.1002/anie.201604708

NOx Trap Three-Way Catalyst (N-TWC) Concept: TWC with NOx Adsorption Properties at Low Temperatures for Cold-Start Emission Control
journal, April 2015

Murata, Yuichiro; Morita, Tomoko; Wada, Katsuji
SAE International Journal of Fuels and Lubricants, Vol. 8, Issue 2
DOI: 10.4271/2015-01-1002

Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3
journal, October 2010

Kwak, Ja Hun; Tonkyn, Russell G.; Kim, Do Heui
Journal of Catalysis, Vol. 275, Issue 2
DOI: 10.1016/j.jcat.2010.07.031

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol
journal, June 2018

Sushkevich, Vitaly L.; Palagin, Dennis; van Bokhoven, Jeroen A.
Angewandte Chemie, Vol. 130, Issue 29
DOI: 10.1002/ange.201802922

Direct Conversion of Methane to Methanol under Mild Conditions over Cu-Zeolites and beyond
journal, January 2017

Tomkins, Patrick; Ranocchiari, Marco; van Bokhoven, Jeroen A.
Accounts of Chemical Research, Vol. 50, Issue 2
DOI: 10.1021/acs.accounts.6b00534

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity
journal, May 2007

Zhan, Bi-Zeng; Iglesia, Enrique
Angewandte Chemie, Vol. 119, Issue 20
DOI: 10.1002/ange.200700128

Solid-State Ion-Exchange of Copper into Zeolites Facilitated by Ammonia at Low Temperature
journal, November 2014

Shwan, Soran; Skoglundh, Magnus; Lundegaard, Lars F.
ACS Catalysis, Vol. 5, Issue 1
DOI: 10.1021/cs5015139

Low-Temperature Pd/Zeolite Passive NO _x Adsorbers: Structure, Performance, and Adsorption Chemistry
journal, July 2017

Zheng, Yang; Kovarik, Libor; Engelhard, Mark H.
The Journal of Physical Chemistry C, Vol. 121, Issue 29
DOI: 10.1021/acs.jpcc.7b04312

Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite
journal, November 2016

Moliner, Manuel; Gabay, Jadeene E.; Kliewer, Chris E.
Journal of the American Chemical Society, Vol. 138, Issue 48
DOI: 10.1021/jacs.6b10169

Zeolite-supported transition metal catalysts by design
journal, October 1992

Sachtler, W. M. H.
Catalysis Today, Vol. 15, Issue 3-4
DOI: 10.1016/0920-5861(92)85007-9

FTIR spectroscopic study of CO adsorption on Pt–H–ZSM-5
journal, June 2005

Chakarova, Kristina; Mihaylov, Mihail; Hadjiivanov, Konstantin
Microporous and Mesoporous Materials, Vol. 81, Issue 1-3
DOI: 10.1016/j.micromeso.2005.01.033

Transition-metal ions in zeolites: the perfect surface sites
journal, January 1988

Klier, Kamil
Langmuir, Vol. 4, Issue 1
DOI: 10.1021/la00079a003

Activation of Hydrogen and Hexane over Pt,H-Mordenite Hydroisomerization Catalysts
journal, May 2009

Lónyi, Ferenc; Kovács, Anita; Szegedi, Ágnes
The Journal of Physical Chemistry C, Vol. 113, Issue 24
DOI: 10.1021/jp810716f

When Gold Is Not Noble: Catalysis by Nanoparticles
journal, April 2003

Haruta, Masatake
The Chemical Record, Vol. 3, Issue 2
DOI: 10.1002/tcr.10053

Effects of hydrothermal aging on NH3-SCR reaction over Cu/zeolites
journal, March 2012

Kwak, Ja Hun; Tran, Diana; Burton, Sarah D.
Journal of Catalysis, Vol. 287
DOI: 10.1016/j.jcat.2011.12.025

Investigations of the Dispersion of Pd in H-ZSM-5
journal, December 1997

Aylor, Adam W.; Lobree, Lisa J.; Reimer, Jeffrey A.
Journal of Catalysis, Vol. 172, Issue 2
DOI: 10.1006/jcat.1997.1893

Metal clusters in zeolites: an intriguing class of catalysts
journal, July 1993

Sachtler, Wolfgang M. H.
Accounts of Chemical Research, Vol. 26, Issue 7
DOI: 10.1021/ar00031a005

Characterization of oxide surfaces and zeolites by carbon monoxide as an IR probe molecule
book, January 2002

Hadjiivanov, Konstantin I.; Vayssilov, Georgi N.
Advances in Catalysis
DOI: 10.1016/S0360-0564(02)47008-3

Crossing the Borders Between Homogeneous and Heterogeneous Catalysis: Developing Recoverable and Reusable Catalytic Systems
journal, April 2008

Corma, Avelino; Garcia, Hermenegildo
Topics in Catalysis, Vol. 48, Issue 1-4
DOI: 10.1007/s11244-008-9056-5

CeO2-M2O3 Passive NO x Adsorbers for Cold Start Applications
journal, December 2016

Jones, Samantha; Ji, Yaying; Bueno-Lopez, Agustín
Emission Control Science and Technology, Vol. 3, Issue 1
DOI: 10.1007/s40825-016-0058-7

A Common Intermediate for N ₂ Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes
journal, August 2013

Kwak, Ja Hun; Lee, Jong H.; Burton, Sarah D.
Angewandte Chemie, Vol. 125, Issue 38
DOI: 10.1002/ange.201303498

Can the state of platinum species be unambiguously determined by the stretching frequency of an adsorbed CO probe molecule?
journal, January 2016

Aleksandrov, Hristiyan A.; Neyman, Konstantin M.; Hadjiivanov, Konstantin I.
Physical Chemistry Chemical Physics, Vol. 18, Issue 32
DOI: 10.1039/C6CP03988J

Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles
journal, April 2018

Liu, Lichen; Corma, Avelino
Chemical Reviews, Vol. 118, Issue 10
DOI: 10.1021/acs.chemrev.7b00776

Recent advances in automotive catalysis for NO _x emission control by small-pore microporous materials
journal, January 2015

Beale, A. M.; Gao, F.; Lezcano-Gonzalez, I.
Chemical Society Reviews, Vol. 44, Issue 20
DOI: 10.1039/C5CS00108K

Synthesis, Modeling, and Catalytic Properties of HY Zeolite-Supported Rhodium Dinitrosyl Complexes
journal, August 2017

Khivantsev, Konstantin; Vityuk, Artem; Aleksandrov, Hristiyan A.
ACS Catalysis, Vol. 7, Issue 9
DOI: 10.1021/acscatal.7b00864

Similar Records in DOE PAGES and OSTI.GOV collections:

Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO _x Adsorbers

Journal Article Khivantsev, Konstantin ; Jaegers, Nicholas R. ; Kovarik, Libor ; ... - Angewandte Chemie

Abstract The majority of harmful atmospheric CO and NO _x emissions are from vehicle exhausts. Although there has been success addressing NO _x emissions at temperatures above 250 °C with selective catalytic reduction technology, emissions during vehicle cold start (when the temperature is below 150 °C), are a major challenge. Herein, we show we can completely eliminate both CO and NO _x emissions simultaneously under realistic exhaust flow, using a highly loaded (2 wt %) atomically dispersed palladium in the extra‐framework positions of the small‐pore chabazite material as a CO and passive NO _x adsorber. Until now, atomicallymore »« less
https://doi.org/10.1002/ange.201809343
Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small-Pore Zeolite SSZ-13: High-Capacity and High-Efficiency Low-Temperature CO and Passive NO_x Adsorbers

Journal Article Khivantsev, Konstantin ; Jaegers, Nicholas R. ; Kovarik, Libor ; ... - Angewandte Chemie (International Edition)

Synthesis of small-pore zeolitic materials with realistic loadings of transition metals atomically dispersed in the micropores has been a formidable challenge. Herein, we demonstrate a new simple and scalable route to high Pd and Pt loadings (>1 wt%) atomically dispersed in the micropores of a small-pore zeolite, SSZ-13. Unlike all previous methods that require addition of expensive transition metal precursor complexes into the synthesis gel and produce low loading of atomically dispersed species, this method does not require any complicated synthetic proce-dures. We determine the factors that govern the stabilization of M(II) species in the micropores of SSZ-13. Using amore »« less
https://doi.org/10.1002/anie.201809343
Molecular Level Understanding of How Oxygen and Carbon Monoxide Improve NOx Storage in Palladium/SSZ-13 Passive NOx Adsorbers: The Role of NO+ and Pd(II)(CO)(NO) Species

Journal Article Khivantsev, Konstantin ; Gao, Feng ; Kovarik, Libor ; ... - Journal of Physical Chemistry C

Addition of molecular oxygen to NO-containing stream improves NOx storage of the Pd/H-SSZ-13. Model Pd/SSZ-13 with high dispersion of Pd ions (0.1 and 1 wt% Pd) was synthesized. The material was characterized with FTIR and cryo-STEM. Adsorption of NO leads to the formation of Pd(II)-NO and Pd(I)-NO complexes as well as NO+ species that replace residual H+ (extra framework) sites. These nitrosyl species are characterized by notable thermal stability, with resistance to decomposition under high vacuum at 200 ºC. Addition of O2 to NO slightly increases the amount of Pd(II)-NO complex with ?NO at ~1865 cm-1 whereas the low frequencymore »« less
https://doi.org/10.1021/acs.jpcc.8b01007
Elucidating the Role of CO in the NO Storage Mechanism on Pd/SSZ-13 with in Situ DRIFTS

Journal Article Song, Inhak ; Khivantsev, Konstantin ; Wang, Yong ; ... - Journal of Physical Chemistry. C

Pd ion exchanged zeolites emerged as promising materials for the adsorption and oxidation of air pollutants. For low-temperature vehicle exhaust, dispersed Pd ions are able to adsorb NO_x even in H₂O-rich exhaust in the presence of carbon monoxide. In order to understand this phenomenon, changes in Pd ligand environment have to be monitored in-situ. Herein, we directly observe the activation of hydrated Pd ion shielded by H₂O into a carbonyl-nitrosyl complex Pd²⁺(NO)(CO) in SSZ-13 zeolite. The subsequent thermal desorption of ligands on Pd²⁺(NO)(CO) complex proceeds to nitrosyl Pd²⁺ rather than to carbonyl Pd²⁺ under various conditions. Thus, CO molecules actmore »« less
https://doi.org/10.1021/acs.jpcc.1c10163

Full Text Available
Palladium/Beta Zeolite Passive NOx Adsorbers (PNA): Clarification of PNA Chemistry and the Effects of CO and Zeolite Crystallite Size on PNA Performance

Journal Article Khivantsev, Konstantin ; Jaegers, Nicholas R. ; Kovarik, Libor ; ... - Applied Catalysis A: General

Model 0.3 wt% and 1 wt% Pd/Beta was synthesized with nano-sized Beta crystals (average size <50 nm) and defect-free large micrometer sized crystals with similar Si/Al ratios ~13 and 15. With the aid of FTIR we reveal the formation of at least two Pd(II)-NO and one Pd(I)-NO complexes upon NO adsorption on those materials under conditions relevant to PNA. Under higher NO pressures at room temperature, we detect the formation of the first palladium (II) dinitrosyl Pd(NO)2 complex, not observed previously on the solid supports or in organometallic compounds. O2 in dry streams promotes NO storage via additional formation ofmore »« less
https://doi.org/10.1016/j.apcata.2018.10.021

Similar Records

Title: Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO x Adsorbers

Abstract

Citation Formats

Selective Catalytic Reduction over Cu/SSZ-13: Linking Homo- and Heterogeneous Catalysis journal, March 2017

Polycarbonyl species in Pt/H–ZSM-5: FTIR spectroscopic study of 12CO–13CO co-adsorption journal, July 2005

Co-ordination chemistry of palladium cations in Pd-H-ZSM-5 as revealed by FTIR spectra of adsorbed and co-adsorbed probe molecules (CO and NO) journal, January 2004

A Common Intermediate for N 2 Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes journal, August 2013

Shape selective and hydrogen spillover approach in the design of sulfur-tolerant hydrogenation catalysts journal, October 2006

Advances in Automobile Emissions Control Catalysis journal, June 2016

Catalytic decomposition of ammonia in a membrane reactor journal, December 1994

Coordinatively Unsaturated Al3+ Centers as Binding Sites for Active Catalyst Phases of Platinum on -Al2O3 journal, September 2009

Low-Temperature Transformation of Methane to Methanol on Pd 1 O 4 Single Sites Anchored on the Internal Surface of Microporous Silicate journal, September 2016

Low Temperature NO Storage of Zeolite Supported Pd for Low Temperature Diesel Engine Emission Control journal, June 2016

Al2O3-based passive NOx adsorbers for low temperature applications journal, July 2015

Coordination and Organometallic Chemistry of Metal−NO Complexes journal, April 2002

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity journal, May 2007

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species journal, December 2009

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol journal, June 2018

Activation of Pd/SSZ-13 catalyst by hydrothermal aging treatment in passive NO adsorption performance at low temperature for cold start application journal, September 2017

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species journal, December 2009

On the hydrothermal stability of Cu/SSZ-13 SCR catalysts journal, June 2018

Molecular Level Understanding of How Oxygen and Carbon Monoxide Improve NO x Storage in Palladium/SSZ-13 Passive NO x Adsorbers: The Role of NO + and Pd(II)(CO)(NO) Species journal, April 2018

Mercaptosilane-Assisted Synthesis of Metal Clusters within Zeolites and Catalytic Consequences of Encapsulation journal, July 2010

Effects of CO on Pd/BEA Passive NOx Adsorbers journal, January 2017

The Adsorption of NO and Reaction of NO with O2on H-, NaH-, CuH-, and Cu-ZSM-5: Anin SituFTIR Investigation journal, November 1996

Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts journal, September 2015

Low-Temperature Transformation of Methane to Methanol on Pd 1 O 4 Single Sites Anchored on the Internal Surface of Microporous Silicate journal, September 2016

NOx Trap Three-Way Catalyst (N-TWC) Concept: TWC with NOx Adsorption Properties at Low Temperatures for Cold-Start Emission Control journal, April 2015

Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3 journal, October 2010

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol journal, June 2018

Direct Conversion of Methane to Methanol under Mild Conditions over Cu-Zeolites and beyond journal, January 2017

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity journal, May 2007

Solid-State Ion-Exchange of Copper into Zeolites Facilitated by Ammonia at Low Temperature journal, November 2014

Low-Temperature Pd/Zeolite Passive NO x Adsorbers: Structure, Performance, and Adsorption Chemistry journal, July 2017

Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite journal, November 2016

Zeolite-supported transition metal catalysts by design journal, October 1992

FTIR spectroscopic study of CO adsorption on Pt–H–ZSM-5 journal, June 2005

Transition-metal ions in zeolites: the perfect surface sites journal, January 1988

Activation of Hydrogen and Hexane over Pt,H-Mordenite Hydroisomerization Catalysts journal, May 2009

When Gold Is Not Noble: Catalysis by Nanoparticles journal, April 2003

Effects of hydrothermal aging on NH3-SCR reaction over Cu/zeolites journal, March 2012

Investigations of the Dispersion of Pd in H-ZSM-5 journal, December 1997

Metal clusters in zeolites: an intriguing class of catalysts journal, July 1993

Characterization of oxide surfaces and zeolites by carbon monoxide as an IR probe molecule book, January 2002

Crossing the Borders Between Homogeneous and Heterogeneous Catalysis: Developing Recoverable and Reusable Catalytic Systems journal, April 2008

CeO2-M2O3 Passive NO x Adsorbers for Cold Start Applications journal, December 2016

A Common Intermediate for N 2 Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes journal, August 2013

Can the state of platinum species be unambiguously determined by the stretching frequency of an adsorbed CO probe molecule? journal, January 2016

Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles journal, April 2018

Recent advances in automotive catalysis for NO x emission control by small-pore microporous materials journal, January 2015

Synthesis, Modeling, and Catalytic Properties of HY Zeolite-Supported Rhodium Dinitrosyl Complexes journal, August 2017

Title: Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small‐Pore Zeolite SSZ‐13: High‐Capacity and High‐Efficiency Low‐Temperature CO and Passive NO _x Adsorbers

Selective Catalytic Reduction over Cu/SSZ-13: Linking Homo- and Heterogeneous Catalysis
journal, March 2017

Polycarbonyl species in Pt/H–ZSM-5: FTIR spectroscopic study of 12CO–13CO co-adsorption
journal, July 2005

Co-ordination chemistry of palladium cations in Pd-H-ZSM-5 as revealed by FTIR spectra of adsorbed and co-adsorbed probe molecules (CO and NO)
journal, January 2004

A Common Intermediate for N ₂ Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes
journal, August 2013

Shape selective and hydrogen spillover approach in the design of sulfur-tolerant hydrogenation catalysts
journal, October 2006

Advances in Automobile Emissions Control Catalysis
journal, June 2016

Catalytic decomposition of ammonia in a membrane reactor
journal, December 1994

Coordinatively Unsaturated Al3+ Centers as Binding Sites for Active Catalyst Phases of Platinum on -Al2O3
journal, September 2009

Low-Temperature Transformation of Methane to Methanol on Pd ₁ O ₄ Single Sites Anchored on the Internal Surface of Microporous Silicate
journal, September 2016

Low Temperature NO Storage of Zeolite Supported Pd for Low Temperature Diesel Engine Emission Control
journal, June 2016

Al2O3-based passive NOx adsorbers for low temperature applications
journal, July 2015

Coordination and Organometallic Chemistry of Metal−NO Complexes
journal, April 2002

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity
journal, May 2007

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species
journal, December 2009

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol
journal, June 2018

Activation of Pd/SSZ-13 catalyst by hydrothermal aging treatment in passive NO adsorption performance at low temperature for cold start application
journal, September 2017

Platinum Sintering on H-ZSM-5 Followed by Chemometrics of CO Adsorption and 2D Pressure-Jump IR Spectroscopy of Adsorbed Species
journal, December 2009

On the hydrothermal stability of Cu/SSZ-13 SCR catalysts
journal, June 2018

Molecular Level Understanding of How Oxygen and Carbon Monoxide Improve NO _x Storage in Palladium/SSZ-13 Passive NO _x Adsorbers: The Role of NO ⁺ and Pd(II)(CO)(NO) Species
journal, April 2018

Mercaptosilane-Assisted Synthesis of Metal Clusters within Zeolites and Catalytic Consequences of Encapsulation
journal, July 2010

Effects of CO on Pd/BEA Passive NOx Adsorbers
journal, January 2017

The Adsorption of NO and Reaction of NO with O2on H-, NaH-, CuH-, and Cu-ZSM-5: Anin SituFTIR Investigation
journal, November 1996

Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
journal, September 2015

Low-Temperature Transformation of Methane to Methanol on Pd ₁ O ₄ Single Sites Anchored on the Internal Surface of Microporous Silicate
journal, September 2016

NOx Trap Three-Way Catalyst (N-TWC) Concept: TWC with NOx Adsorption Properties at Low Temperatures for Cold-Start Emission Control
journal, April 2015

Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3
journal, October 2010

The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol
journal, June 2018

Direct Conversion of Methane to Methanol under Mild Conditions over Cu-Zeolites and beyond
journal, January 2017

RuO2 Clusters within LTA Zeolite Cages: Consequences of Encapsulation on Catalytic Reactivity and Selectivity
journal, May 2007

Solid-State Ion-Exchange of Copper into Zeolites Facilitated by Ammonia at Low Temperature
journal, November 2014

Low-Temperature Pd/Zeolite Passive NO _x Adsorbers: Structure, Performance, and Adsorption Chemistry
journal, July 2017

Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite
journal, November 2016

Zeolite-supported transition metal catalysts by design
journal, October 1992

FTIR spectroscopic study of CO adsorption on Pt–H–ZSM-5
journal, June 2005

Transition-metal ions in zeolites: the perfect surface sites
journal, January 1988

Activation of Hydrogen and Hexane over Pt,H-Mordenite Hydroisomerization Catalysts
journal, May 2009

When Gold Is Not Noble: Catalysis by Nanoparticles
journal, April 2003

Effects of hydrothermal aging on NH3-SCR reaction over Cu/zeolites
journal, March 2012

Investigations of the Dispersion of Pd in H-ZSM-5
journal, December 1997

Metal clusters in zeolites: an intriguing class of catalysts
journal, July 1993

Characterization of oxide surfaces and zeolites by carbon monoxide as an IR probe molecule
book, January 2002

Crossing the Borders Between Homogeneous and Heterogeneous Catalysis: Developing Recoverable and Reusable Catalytic Systems
journal, April 2008

CeO2-M2O3 Passive NO x Adsorbers for Cold Start Applications
journal, December 2016

A Common Intermediate for N ₂ Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes
journal, August 2013

Can the state of platinum species be unambiguously determined by the stretching frequency of an adsorbed CO probe molecule?
journal, January 2016

Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles
journal, April 2018

Recent advances in automotive catalysis for NO _x emission control by small-pore microporous materials
journal, January 2015

Synthesis, Modeling, and Catalytic Properties of HY Zeolite-Supported Rhodium Dinitrosyl Complexes
journal, August 2017