Insights into palladium poisoning of Cu/SSZ-13 selective catalytic reduction catalysts

Wu, Yiqing; Wang, Yilin; Walter, Eric D.; Rappé, Kenneth G.; Wang, Yong; Gao, Feng

doi:10.1016/j.apcatb.2023.122673

Insights into palladium poisoning of Cu/SSZ-13 selective catalytic reduction catalysts

Journal Article · Thu Mar 23 00:00:00 UTC 2023 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2023.122673· OSTI ID:1969553

Wu, Yiqing ^[1]; Wang, Yilin ^[1]; ^[1]; ^[1]; Wang, Yong ^[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)

Here, the impacts of Pd poisoning to the activity, selectivity, and hydrothermal stability of Cu/SSZ-13 selective catalytic reduction (SCR) catalysts are reported. Pd lowers DeNOx efficiency of Cu/SSZ-13 via two mechanisms: (1) displacing SCR active sites in the form of isolated Pd-ions, and (2) catalyzing non-selective NH₃ oxidation in the form of PdO. The first mechanism works by the diffusion of isolated Pd-ions into chabazite cages to displace ZCu^IIOH SCR active species, and it occurs on Cu/SSZ-13 catalysts with and without external surface CuO clusters in similar fashion. In contrast, the second mechanism works differently with and without external surface CuO clusters. For Cu/SSZ-13 catalyst without external CuO clusters (i.e., primarily isolated Cu-ions), PdO leads to significant decrease of DeNOx efficiency at reaction temperatures above ~400°C due to its non-selective NH₃ oxidation activity at high temperatures. However, this poisoning effect becomes much less impactful on Cu/SSZ-13 catalyst containing CuO clusters. This is due to the formation of CuO-PdO solid solution via interactions between CuO and PdO, which reduces non-selective NH₃ oxidation potential. Furthermore, this solid solution formation even mitigates adverse effects caused by hydrothermal aging. Hence, the poisoning effects of Pd are closely related to Cu speciation and spatial distribution of a Cu/SSZ-13 catalyst. Finally, this study suggests a strategy in eliminating Pd poisoning, that is, the introduction of an oxide phase that effectively traps PdO but does not adversely influence SCR.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1969553

Alternate ID(s):: OSTI ID: 1967511

Report Number(s):: PNNL-SA-177938

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 331; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

The role of palladium in a hydrogen economy Adams, Brian D.; Chen, Aicheng Materials Today, Vol. 14, Issue 6 https://doi.org/10.1016/S1369-7021(11)70143-2	journal	June 2011
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
Passive NOx adsorber: An overview of catalyst performance and reaction chemistry Gu, Yuntao; Epling, William S. Applied Catalysis A: General, Vol. 570 https://doi.org/10.1016/j.apcata.2018.10.036	journal	January 2019
Chemical deactivation of Cu-SSZ-13 ammonia selective catalytic reduction (NH3-SCR) systems Lezcano-Gonzalez, I.; Deka, U.; van der Bij, H. E. Applied Catalysis B: Environmental, Vol. 154-155 https://doi.org/10.1016/j.apcatb.2014.02.037	journal	July 2014
Synthesis and evaluation of Cu/SAPO-34 catalysts for NH3-SCR 2: Solid-state ion exchange and one-pot synthesis Gao, Feng; Walter, Eric D.; Washton, Nancy M. Applied Catalysis B: Environmental, Vol. 162 https://doi.org/10.1016/j.apcatb.2014.07.029	journal	January 2015
Bimetallic Pd–Cu catalysts for selective CO2 hydrogenation to methanol Jiang, Xiao; Koizumi, Naoto; Guo, Xinwen Applied Catalysis B: Environmental, Vol. 170-171 https://doi.org/10.1016/j.apcatb.2015.01.010	journal	July 2015
Insight of platinum poisoning Cu/SAPO-34 during NH3-SCR and its promotion on catalysts regeneration after hydrothermal treatment Yu, Tie; Xu, Minhong; Huang, Yu Applied Catalysis B: Environmental, Vol. 204 https://doi.org/10.1016/j.apcatb.2016.12.007	journal	May 2017
Volatilisation and subsequent deposition of platinum oxides from diesel oxidation catalysts Leistner, Kirsten; Gonzalez Braga, Carolina; Kumar, Ashok Applied Catalysis B: Environmental, Vol. 241 https://doi.org/10.1016/j.apcatb.2018.09.022	journal	February 2019
Enhancement of high-temperature selectivity on Cu-SSZ-13 towards NH3-SCR reaction from highly dispersed ZrO2 Peng, Bo; Rappé, Kenneth G.; Cui, Yanran Applied Catalysis B: Environmental, Vol. 263 https://doi.org/10.1016/j.apcatb.2019.118359	journal	April 2020
A comparative study of the activity and hydrothermal stability of Al-rich Cu-SSZ-39 and Cu-SSZ-13 Shan, Yulong; Shan, Wenpo; Shi, Xiaoyan Applied Catalysis B: Environmental, Vol. 264 https://doi.org/10.1016/j.apcatb.2019.118511	journal	May 2020
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
Selective oxidation of ammonia to nitrogen on bi-functional Cu–SSZ-13 and Pt/Al2O3 monolith catalyst Shrestha, Sachi; Harold, Michael P.; Kamasamudram, Krishna Catalysis Today, Vol. 267 https://doi.org/10.1016/j.cattod.2015.11.035	journal	June 2016
Electrochemical study of carbon dioxide reduction at copper–palladium nanoparticles: Influence of the bimetallic composition in the CO poisoning tolerance Torralba, E.; Blanchard, N.; Cachet-Vivier, C. Electrochimica Acta, Vol. 354 https://doi.org/10.1016/j.electacta.2020.136739	journal	September 2020
Hydrothermal stability of CuSSZ13 for reducing NOx by NH3 Kim, Young Jin; Lee, Jun Kyu; Min, Kyung Myung Journal of Catalysis, Vol. 311 https://doi.org/10.1016/j.jcat.2013.12.012	journal	March 2014
Effects of Si/Al ratio on Cu/SSZ-13 NH3-SCR catalysts: Implications for the active Cu species and the roles of Brønsted acidity Gao, Feng; Washton, Nancy M.; Wang, Yilin Journal of Catalysis, Vol. 331 https://doi.org/10.1016/j.jcat.2015.08.004	journal	November 2015
Revisiting effects of alkali metal and alkaline earth co-cation additives to Cu/SSZ-13 selective catalytic reduction catalysts Cui, Yanran; Wang, Yilin; Mei, Donghai Journal of Catalysis, Vol. 378 https://doi.org/10.1016/j.jcat.2019.08.028	journal	October 2019
Excellent Activity and Selectivity of One-Pot Synthesized Cu–SSZ-13 Catalyst in the Selective Catalytic Oxidation of Ammonia to Nitrogen Zhang, Tao; Chang, Huazhen; You, Yanchen Environmental Science & Technology, Vol. 52, Issue 8 https://doi.org/10.1021/acs.est.8b00267	journal	March 2018
Quantitative Cu Counting Methodologies for Cu/SSZ-13 Selective Catalytic Reduction Catalysts by Electron Paramagnetic Resonance Spectroscopy Zhang, Yani; Wu, Yiqing; Peng, Yue The Journal of Physical Chemistry C, Vol. 124, Issue 51 https://doi.org/10.1021/acs.jpcc.0c07971	journal	December 2020
Effect of Cu Concentration on the Selective Catalytic Reduction of NO with Ammonia for Aluminosilicate Zeolite SSZ-13 Catalysts Zhou, Shuo; Tang, Fushun; Wang, Hui The Journal of Physical Chemistry C, Vol. 125, Issue 27 https://doi.org/10.1021/acs.jpcc.1c04055	journal	July 2021
Selective Catalytic Reduction of NO _x with NH ₃ over Cu/SSZ-13: Elucidating Dynamics of Cu Active Sites with In Situ UV–Vis Spectroscopy and DFT Calculations Zhang, Yani; Zhang, Jun; Wang, Houlin The Journal of Physical Chemistry C, Vol. 126, Issue 20 https://doi.org/10.1021/acs.jpcc.2c01268	journal	May 2022
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
Autoreduction of Copper in Zeolites: Role of Topology, Si/Al Ratio, and Copper Loading Sushkevich, Vitaly L.; Smirnov, Andrei V.; van Bokhoven, Jeroen A. The Journal of Physical Chemistry C, Vol. 123, Issue 15 https://doi.org/10.1021/acs.jpcc.9b00986	journal	March 2019
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
Probing Active-Site Relocation in Cu/SSZ-13 SCR Catalysts during Hydrothermal Aging by In Situ EPR Spectroscopy, Kinetics Studies, and DFT Calculations Zhang, Yani; Peng, Yue; Li, Junhua ACS Catalysis, Vol. 10, Issue 16 https://doi.org/10.1021/acscatal.0c01590	journal	June 2020
Influence of ZCuOH, Z ₂ Cu, and Extraframework Cu _x O _y Species in Cu-SSZ-13 on N ₂ O Formation during the Selective Catalytic Reduction of NO _x with NH ₃ Shih, Arthur J.; González, Juan M.; Khurana, Ishant ACS Catalysis, Vol. 11, Issue 16 https://doi.org/10.1021/acscatal.1c01871	journal	August 2021
Effects of Alkali and Alkaline Earth Cocations on the Activity and Hydrothermal Stability of Cu/SSZ-13 NH ₃ –SCR Catalysts Gao, Feng; Wang, Yilin; Washton, Nancy M. ACS Catalysis, Vol. 5, Issue 11 https://doi.org/10.1021/acscatal.5b01621	journal	October 2015
Toward Rational Design of Cu/SSZ-13 Selective Catalytic Reduction Catalysts: Implications from Atomic-Level Understanding of Hydrothermal Stability Song, James; Wang, Yilin; Walter, Eric D. ACS Catalysis, Vol. 7, Issue 12 https://doi.org/10.1021/acscatal.7b03020	journal	November 2017
Enhanced Selective Oxidation of Ammonia in a Pt/Al₂O₃@Cu/ZSM-5 Core–Shell Catalyst Ghosh, Rajat Subhra; Le, Thuy T.; Terlier, Tanguy ACS Catalysis, Vol. 10, Issue 6 https://doi.org/10.1021/acscatal.9b04288	journal	February 2020
Spillover in Heterogeneous Catalysis Conner, W. Curtis.; Falconer, John L. Chemical Reviews, Vol. 95, Issue 3 https://doi.org/10.1021/cr00035a014	journal	May 1995
NO Chemisorption on Cu/SSZ-13: A Comparative Study from Infrared Spectroscopy and DFT Calculations Zhang, Renqin; McEwen, Jean-Sabin; Kollár, Márton ACS Catalysis, Vol. 4, Issue 11 https://doi.org/10.1021/cs500563s	journal	October 2014
Structure and Reactivity of Oxygen-Bridged Diamino Dicopper(II) Complexes in Cu-Ion-Exchanged Chabazite Catalyst for NH ₃ -Mediated Selective Catalytic Reduction Negri, Chiara; Selleri, Tommaso; Borfecchia, Elisa Journal of the American Chemical Society, Vol. 142, Issue 37 https://doi.org/10.1021/jacs.0c06270	journal	August 2020
Rate Controlling in Low-Temperature Standard NH₃-SCR: Implications from Operando EPR Spectroscopy and Reaction Kinetics Wu, Yiqing; Ma, Yue; Wang, Yilin Journal of the American Chemical Society, Vol. 144, Issue 22 https://doi.org/10.1021/jacs.2c01933	journal	May 2022
The Structure of Monomeric Hydroxo-Cu^II Species in Cu-CHA. A Quantitative Assessment Bruzzese, Paolo Cleto; Salvadori, Enrico; Civalleri, Bartolomeo Journal of the American Chemical Society, Vol. 144, Issue 29 https://doi.org/10.1021/jacs.2c06037	journal	July 2022
Catalysis in a Cage: Condition-Dependent Speciation and Dynamics of Exchanged Cu Cations in SSZ-13 Zeolites Paolucci, Christopher; Parekh, Atish A.; Khurana, Ishant Journal of the American Chemical Society, Vol. 138, Issue 18 https://doi.org/10.1021/jacs.6b02651	journal	April 2016
Selective Catalytic Reduction over Cu/SSZ-13: Linking Homo- and Heterogeneous Catalysis Gao, Feng; Mei, Donghai; Wang, Yilin Journal of the American Chemical Society, Vol. 139, Issue 13 https://doi.org/10.1021/jacs.7b01128	journal	March 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
Characterization of Copper Palladium Oxide Solid Solutions by X-ray Diffraction, X-ray Photoelectron Spectroscopy, and Auger Electron Spectroscopy Christensen, Gregory L.; Langell, Marjorie A. The Journal of Physical Chemistry C, Vol. 117, Issue 14 https://doi.org/10.1021/jp310344r	journal	March 2013
Coordination Environment of Copper Sites in Cu-CHA Zeolite Investigated by Electron Paramagnetic Resonance Godiksen, Anita; Stappen, Frederick N.; Vennestrøm, Peter N. R. The Journal of Physical Chemistry C, Vol. 118, Issue 40 https://doi.org/10.1021/jp5065616	journal	September 2014
Recent advances in automotive catalysis for NO _x emission control by small-pore microporous materials Beale, A. M.; Gao, F.; Lezcano-Gonzalez, I. Chemical Society Reviews, Vol. 44, Issue 20 https://doi.org/10.1039/C5CS00108K	journal	January 2015
Effect of the hydrothermal aging temperature and Cu/Al ratio on the hydrothermal stability of CuSSZ-13 catalysts for NH ₃ -SCR Han, Shuai; Ye, Qing; Cheng, Shuiyuan Catalysis Science & Technology, Vol. 7, Issue 3 https://doi.org/10.1039/C6CY02555B	journal	January 2017
Cu-CHA – a model system for applied selective redox catalysis Borfecchia, Elisa; Beato, Pablo; Svelle, Stian Chemical Society Reviews, Vol. 47, Issue 22 https://doi.org/10.1039/C8CS00373D	journal	January 2018
Two different cationic positions in Cu-SSZ-13? Hun Kwak, Ja; Zhu, Haiyang; Lee, Jong H. Chemical Communications, Vol. 48, Issue 39 https://doi.org/10.1039/c2cc31184d	journal	January 2012
Dynamic multinuclear sites formed by mobilized copper ions in NO _x selective catalytic reduction Paolucci, Christopher; Khurana, Ishant; Parekh, Atish A. Science, Vol. 357, Issue 6354 https://doi.org/10.1126/science.aan5630	journal	August 2017

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Insights into palladium poisoning of Cu/SSZ-13 selective catalytic reduction catalysts

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