Elucidating the Role of CO in the NO Storage Mechanism on Pd/SSZ-13 with in Situ DRIFTS

Song, Inhak; Khivantsev, Konstantin; Wang, Yong; Szanyi, János

doi:10.1021/acs.jpcc.1c10163

Title: Elucidating the Role of CO in the NO Storage Mechanism on Pd/SSZ-13 with in Situ DRIFTS

Journal Article · 13 January 2022 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.1c10163 · OSTI ID:1842285

Song, Inhak ^[1];

^[1];

^[2];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Institute for Integrated Catalysis; Washington State Univ., Pullman, WA (United States)

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 act as additional ligands to provide alternative pathway through Pd²⁺(NO)(CO) complex with lower energy barrier for accelerating NO adsorption on hydrated Pd²⁺ ion, which is kinetically limited in the absence of CO. We further demonstrate that hydration of Pd ions in the zeolite is a prerequisite for CO-induced reduction of Pd ions to metallic Pd. The reduction of Pd ions by CO is limited under dry conditions even at a high temperature of 500°C, while water makes it possible at near RT. However, the primary NO adsorption sites are Pd²⁺ ions even in gases containing CO and water. These findings clarify additional mechanistic aspects of the passive NO_x adsorption (PNA) process and will help extend the NOx adsorption chemistry in zeolite-based adsorbers to practical applications.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1842285

Report Number(s):: PNNL-SA--168814

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 3 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (49)

Economizing on Precious Metals in Three‐Way Catalysts: Thermally Stable and Highly Active Single‐Atom Rhodium on Ceria for NO Abatement under Dry and Industrially Relevant Conditions** Khivantsev, Konstantin; Vargas, Carlos Garcia; Tian, Jinshu Angewandte Chemie, Vol. 133, Issue 1 https://doi.org/10.1002/ange.202010815	journal	October 2020
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 Angewandte Chemie International Edition, Vol. 57, Issue 51 https://doi.org/10.1002/anie.201809343	journal	November 2018
Palladium/Ferrierite versus Palladium/SSZ‐13 Passive NOx Adsorbers: Adsorbate‐Controlled Location of Atomically Dispersed Palladium(II) in Ferrierite Determines High Activity and Stability** Khivantsev, Konstantin; Wei, Xinyi; Kovarik, Libor Angewandte Chemie International Edition, Vol. 61, Issue 3 https://doi.org/10.1002/anie.202107554	journal	December 2021
Investigations of the Dispersion of Pd in H-ZSM-5 Aylor, Adam W.; Lobree, Lisa J.; Reimer, Jeffrey A. Journal of Catalysis, Vol. 172, Issue 2 https://doi.org/10.1006/jcat.1997.1893	journal	December 1997
Structure, Distribution, and Properties of Co Ions in Ferrierite Revealed by FTIR, UV–Vis, and EXAFS Sobalı́k, Zdeněk; Dědeček, Jiřı́; Kaucký, Dalibor Journal of Catalysis, Vol. 194, Issue 2 https://doi.org/10.1006/jcat.2000.2926	journal	September 2000
NO x uptake mechanism on Pt/BaO/Al2O3 catalysts Kwak, Ja Hun; Kim, Do Heui; Szailer, Tamás Catalysis Letters, Vol. 111, Issue 3-4 https://doi.org/10.1007/s10562-006-0153-4	journal	November 2006
Low Temperature NO Storage of Zeolite Supported Pd for Low Temperature Diesel Engine Emission Control Chen, Hai-Ying; Collier, Jillian E.; Liu, Dongxia Catalysis Letters, Vol. 146, Issue 9 https://doi.org/10.1007/s10562-016-1794-6	journal	June 2016
Current Understanding of Cu-Exchanged Chabazite Molecular Sieves for Use as Commercial Diesel Engine DeNOx Catalysts Gao, Feng; Kwak, Ja Hun; Szanyi, Janos Topics in Catalysis, Vol. 56, Issue 15-17 https://doi.org/10.1007/s11244-013-0145-8	journal	August 2013
Comparison of NOx Adsorption/Desorption Behaviors over Pd/CeO2 and Pd/SSZ-13 as Passive NOx Adsorbers for Cold Start Application Kim, Yongwoo; Hwang, Sungha; Lee, Jaeha Emission Control Science and Technology, Vol. 5, Issue 2 https://doi.org/10.1007/s40825-019-00119-0	journal	April 2019
Palladium/Zeolite Low Temperature Passive NOx Adsorbers (PNA): Structure-Adsorption Property Relationships for Hydrothermally Aged PNA Materials Khivantsev, Konstantin; Jaegers, Nicholas R.; Kovarik, Libor Emission Control Science and Technology, Vol. 6, Issue 2 https://doi.org/10.1007/s40825-019-00139-w	journal	September 2019
An in situ Fourier transform infrared studyof zeolitic vibrations: Dehydration, deammoniation, and reammoniation of ion-exchanged Y zeolites Jacobs, W. P. J. H.; van Wolput, J. H. M. C.; van Santen, R. A. Zeolites, Vol. 13, Issue 3 https://doi.org/10.1016/S0144-2449(05)80274-X	journal	March 1993
Oxidative redispersion of palladium and formation of PdO particles in NaY Homeyer, S. T.; Sachtler, W. M. H. Applied Catalysis, Vol. 54, Issue 1 https://doi.org/10.1016/S0166-9834(00)82364-7	journal	September 1989
On the hydrothermal stability of Cu/SSZ-13 SCR catalysts Gao, Feng; Szanyi, János Applied Catalysis A: General, Vol. 560 https://doi.org/10.1016/j.apcata.2018.04.040	journal	June 2018
Effect of reduction treatments (H2 vs. CO) on the NO adsorption ability and the physicochemical properties of Pd/SSZ-13 passive NOx adsorber for cold start application Ryou, YoungSeok; Lee, Jaeha; Kim, Yongwoo Applied Catalysis A: General, Vol. 569 https://doi.org/10.1016/j.apcata.2018.10.016	journal	January 2019
Palladium/Beta zeolite passive NOx adsorbers (PNA): Clarification of PNA chemistry and the effects of CO and zeolite crystallite size on PNA performance Khivantsev, Konstantin; Jaegers, Nicholas R.; Kovarik, Libor Applied Catalysis A: General, Vol. 569 https://doi.org/10.1016/j.apcata.2018.10.021	journal	January 2019
Mechanistic insight into the passive NOx adsorption in the highly dispersed Pd/HBEA zeolite Mei, Donghai; Gao, Feng; Szanyi, Janos Applied Catalysis A: General, Vol. 569 https://doi.org/10.1016/j.apcata.2018.10.037	journal	January 2019
Activation of Pd/SSZ-13 catalyst by hydrothermal aging treatment in passive NO adsorption performance at low temperature for cold start application Ryou, YoungSeok; Lee, Jaeha; Cho, Sung June Applied Catalysis B: Environmental, Vol. 212 https://doi.org/10.1016/j.apcatb.2017.04.077	journal	September 2017
Investigation of the active sites and optimum Pd/Al of Pd/ZSM–5 passive NO adsorbers for the cold-start application: Evidence of isolated-Pd species obtained after a high-temperature thermal treatment Lee, Jaeha; Ryou, YoungSeok; Cho, Sung June Applied Catalysis B: Environmental, Vol. 226 https://doi.org/10.1016/j.apcatb.2017.12.031	journal	June 2018
Improving NOx storage and CO oxidation abilities of Pd/SSZ-13 by increasing its hydrophobicity Lee, Jaeha; Kim, Jonghyun; Kim, Yongwoo Applied Catalysis B: Environmental, Vol. 277 https://doi.org/10.1016/j.apcatb.2020.119190	journal	November 2020
The superior hydrothermal stability of Pd/SSZ-39 in low temperature passive NOx adsorption (PNA) and methane combustion Khivantsev, Konstantin; Jaegers, Nicholas R.; Kovarik, Libor Applied Catalysis B: Environmental, Vol. 280 https://doi.org/10.1016/j.apcatb.2020.119449	journal	January 2021
Mechanistic insight in NO trapping on Pd/Chabazite systems for the low-temperature NOx removal from Diesel exhausts Villamaina, Roberta; Iacobone, Umberto; Nova, Isabella Applied Catalysis B: Environmental, Vol. 284 https://doi.org/10.1016/j.apcatb.2020.119724	journal	May 2021
Investigation of crystal size effect on the NOx storage performance of Pd/SSZ-13 passive NOx adsorbers Chen, Zexiang; Wang, Mingdong; Wang, Jun Applied Catalysis B: Environmental, Vol. 291 https://doi.org/10.1016/j.apcatb.2021.120026	journal	August 2021
A comparative kinetics study between Cu/SSZ-13 and Fe/SSZ-13 SCR catalysts Gao, Feng; Wang, Yilin; Kollár, Márton Catalysis Today, Vol. 258 https://doi.org/10.1016/j.cattod.2015.01.025	journal	December 2015
Effect of sulfur aging and regeneration on low temperature NO adsorption over hydrothermally treated Pd/CeO 2 and Pd/Ce 0.58 Zr 0.42 O 2 catalysts Ryou, YoungSeok; Lee, Jaeha; Lee, Hyokyoung Catalysis Today, Vol. 297 https://doi.org/10.1016/j.cattod.2017.06.035	journal	November 2017
NOx uptake and release on Pd/SSZ-13: Impact Of Feed composition and temperature Gupta, Abhay; Kang, Sung Bong; Harold, Michael P. Catalysis Today, Vol. 360 https://doi.org/10.1016/j.cattod.2020.01.018	journal	January 2021
Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3 Kwak, Ja Hun; Tonkyn, Russell G.; Kim, Do Heui Journal of Catalysis, Vol. 275, Issue 2 https://doi.org/10.1016/j.jcat.2010.07.031	journal	October 2010
Following the movement of Cu ions in a SSZ-13 zeolite during dehydration, reduction and adsorption: A combined in situ TP-XRD, XANES/DRIFTS study Kwak, Ja Hun; Varga, Tamás; Peden, Charles H. F. Journal of Catalysis, Vol. 314 https://doi.org/10.1016/j.jcat.2014.03.003	journal	May 2014
Structural Interconversion between Agglomerated Palladium Domains and Mononuclear Pd(II) Cations in Chabazite Zeolites Lardinois, Trevor M.; Bates, Jason S.; Lippie, Harrison H. Chemistry of Materials, Vol. 33, Issue 5 https://doi.org/10.1021/acs.chemmater.0c04465	journal	February 2021
Low-Temperature Pd/Zeolite Passive NO _x Adsorbers: Structure, Performance, and Adsorption Chemistry Zheng, Yang; Kovarik, Libor; Engelhard, Mark H. The Journal of Physical Chemistry C, Vol. 121, Issue 29 https://doi.org/10.1021/acs.jpcc.7b04312	journal	July 2017
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 Khivantsev, Konstantin; Gao, Feng; Kovarik, Libor The Journal of Physical Chemistry C, Vol. 122, Issue 20 https://doi.org/10.1021/acs.jpcc.8b01007	journal	April 2018
Stabilization of Super Electrophilic Pd ⁺² Cations in Small-Pore SSZ-13 Zeolite Khivantsev, Konstantin; Jaegers, Nicholas R.; Koleva, Iskra Z. The Journal of Physical Chemistry C, Vol. 124, Issue 1 https://doi.org/10.1021/acs.jpcc.9b06760	journal	December 2019
Theoretical and Spectroscopic Evidence of the Dynamic Nature of Copper Active Sites in Cu-CHA Catalysts under Selective Catalytic Reduction (NH ₃ –SCR–NO _x ) Conditions Millan, Reisel; Cnudde, Pieter; Hoffman, Alexander E. J. The Journal of Physical Chemistry Letters, Vol. 11, Issue 23 https://doi.org/10.1021/acs.jpclett.0c03020	journal	November 2020
Mobility of Cu Ions in Cu-SSZ-13 Determines the Reactivity of Selective Catalytic Reduction of NO _x with NH ₃ Lee, Hwangho; Song, Inhak; Jeon, Se Won The Journal of Physical Chemistry Letters, Vol. 12, Issue 12 https://doi.org/10.1021/acs.jpclett.1c00181	journal	March 2021
Controlling Catalytic Selectivity Mediated by Stabilization of Reactive Intermediates in Small-Pore Environments: A Study of Mn/TiO ₂ in the NH ₃ -SCR Reaction Song, Inhak; Lee, Hwangho; Jeon, Se Won ACS Catalysis, Vol. 10, Issue 20 https://doi.org/10.1021/acscatal.0c03154	journal	September 2020
Condition-Dependent Pd Speciation and NO Adsorption in Pd/Zeolites Mandal, Keka; Gu, Yuntao; Westendorff, Karl S. ACS Catalysis, Vol. 10, Issue 21 https://doi.org/10.1021/acscatal.0c03585	journal	September 2020
CH ₄ Oxidation Activity in Pd and Pt–Pd Bimetallic Catalysts: Correlation with Surface PdO _x Quantified from the DRIFTS Study Jang, Eun Jeong; Lee, Jaekyoung; Oh, Dong Gun ACS Catalysis, Vol. 11, Issue 10 https://doi.org/10.1021/acscatal.1c00156	journal	April 2021
Synthesis, Modeling, and Catalytic Properties of HY Zeolite-Supported Rhodium Dinitrosyl Complexes Khivantsev, Konstantin; Vityuk, Artem; Aleksandrov, Hristiyan A. ACS Catalysis, Vol. 7, Issue 9 https://doi.org/10.1021/acscatal.7b00864	journal	August 2017
Onset of High Methane Combustion Rates over Supported Palladium Catalysts: From Isolated Pd Cations to PdO Nanoparticles Cui, Yanran; Zhu Chen, Johnny; Peng, Bo JACS Au, Vol. 1, Issue 4 https://doi.org/10.1021/jacsau.0c00109	journal	March 2021
Mobility and Reactivity of Cu ⁺ Species in Cu-CHA Catalysts under NH ₃ -SCR-NOx Reaction Conditions: Insights from AIMD Simulations Millan, Reisel; Cnudde, Pieter; van Speybroeck, Veronique JACS Au, Vol. 1, Issue 10 https://doi.org/10.1021/jacsau.1c00337	journal	September 2021
Regulation of the Dispersion of PdO through the Interaction with Acid Sites of Zeolite Studied by Extended X-ray Absorption Fine Structure Okumura, Kazu; Niwa, Miki The Journal of Physical Chemistry B, Vol. 104, Issue 41 https://doi.org/10.1021/jp001543y	journal	October 2000
In-Situ QXAFS Studies on the Dynamic Coalescence and Dispersion Processes of Pd in the USY Zeolite Okumura, Kazu; Kato, Kazuo; Sanada, Takashi The Journal of Physical Chemistry C, Vol. 111, Issue 39 https://doi.org/10.1021/jp073874h	journal	September 2007
Dynamic in situ observation of rapid size and shape change of supported Pd nanoparticles during CO/NO cycling Newton, Mark A.; Belver-Coldeira, Carolina; Martínez-Arias, Arturo Nature Materials, Vol. 6, Issue 7 https://doi.org/10.1038/nmat1924	journal	May 2007
Unraveling the mysterious failure of Cu/SAPO-34 selective catalytic reduction catalysts Wang, Aiyong; Chen, Ying; Walter, Eric D. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09021-3	journal	March 2019
Tuning Pt-CeO2 interactions by high-temperature vapor-phase synthesis for improved reducibility of lattice oxygen Pereira-Hernández, Xavier Isidro; DeLaRiva, Andrew; Muravev, Valery Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09308-5	journal	March 2019
Simple physical mixing of zeolite prevents sulfur deactivation of vanadia catalysts for NOx removal Song, Inhak; Lee, Hwangho; Jeon, Se Won Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-21228-x	journal	February 2021
The impact of automotive catalysis on the United Nations sustainable development goals Wang, Aiyong; Olsson, Louise Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0318-3	journal	July 2019
Uniform synthesis of palladium species confined in a small-pore zeolite via full ion-exchange investigated by cryogenic electron microscopy Kim, Yongwoo; Sung, Jongbaek; Kang, Sungsu Journal of Materials Chemistry A, Vol. 9, Issue 35 https://doi.org/10.1039/D1TA00468A	journal	January 2021
Characterization of Cu-SSZ-13 NH3 SCR catalysts: an in situ FTIR study Szanyi, János; Kwak, Ja Hun; Zhu, Haiyang Physical Chemistry Chemical Physics, Vol. 15, Issue 7 https://doi.org/10.1039/c2cp43467a	journal	January 2013
On the Nature of Water Bound to a Solid Acid Catalyst Smith, L.; Cheetham, A. K.; Morris, R. E. Science, Vol. 271, Issue 5250 https://doi.org/10.1126/science.271.5250.799	journal	February 1996

Similar Records

Stabilization of Super Electrophilic Pd⁺² Cations in Small-Pore SSZ-13 Zeolite

Journal Article · 2019 · Journal of Physical Chemistry. C · OSTI ID:1617560

Khivantsev, Konstantin; Jaegers, Nicholas R.; Koleva, Iskra Z.; +7 more

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 · 2018 · Journal of Physical Chemistry C · OSTI ID:1577856

Khivantsev, Konstantin; Gao, Feng; Kovarik, Libor; +2 more

Increasing Al-Pair Abundance in SSZ-13 Zeolite via Zeolite Synthesis in the Presence of Alkaline Earth Metal Hydroxide Produces Hydrothermally Stable Co-, Cu- and Pd-SSZ-13 Materials

Journal Article · 2024 · Catalysts · OSTI ID:2396881

Khivantsev, Konstantin; Derewinski, Miroslaw A.; Kovarik, Libor; +8 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Elucidating the Role of CO in the NO Storage Mechanism on Pd/SSZ-13 with in Situ DRIFTS

Citation Formats

References (49)

Similar Records

Related Subjects