Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts

Gao, Feng; Peden, Charles H. F.

doi:10.3390/catal8040140

Title: Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts

Abstract

Cu/SSZ-13 Selective Catalytic Reduction (SCR) catalysts have been extensively studied for the past five-plus years. New and exciting fundamental and applied science has appeared in the literature quite frequently over this time. In this short review, a few topics specifically focused on a molecular-level understanding of this catalyst are summarized: (1) The nature of the active sites and, in particular, their transformations under varying reaction conditions that include dehydration, the presence of the various SCR reactants and hydrothermal aging; (2) Discussions of standard and fast SCR reaction mechanisms. Considerable progress has been made, especially in the last couple of years, on standard SCR mechanisms. In contrast, mechanisms for fast SCR are much less understood. Possible reaction paths are hypothesized for this latter case to stimulate further investigations; (3) Discussions of rational catalyst design based on new knowledge obtained regarding catalyst stability, overall catalytic performance and mechanistic catalytic chemistry.

Authors:

Gao, Feng ^[1]; Peden, Charles H. F. ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Institute for Integrated Catalysis

Publication Date:: Sat Mar 31 00:00:00 EDT 2018

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

OSTI Identifier:: 1457764

Report Number(s):: PNNL-SA-132856
Journal ID: ISSN 2073-4344; CATACJ; PII: catal8040140

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Catalysts

Additional Journal Information:: Journal Volume: 8; Journal Issue: 4; Journal ID: ISSN 2073-4344

Publisher:: MDPI

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; selective catalytic reduction (SCR); zeolite; Cu/SSZ-13; reaction mechanisms; hydrothermal stability; standard SCR; fast SCR

Citation Formats


                    Gao, Feng, and Peden, Charles H. F. Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts.  United States: N. p., 2018. 
Web.  doi:10.3390/catal8040140.

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                    Gao, Feng, & Peden, Charles H. F. Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts.  United States.  https://doi.org/10.3390/catal8040140

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                    Gao, Feng, and Peden, Charles H. F. Sat .  
"Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts".  United States.  https://doi.org/10.3390/catal8040140.  https://www.osti.gov/servlets/purl/1457764.

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@article{osti_1457764,

  title        = {Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts},

  author       = {Gao, Feng and Peden, Charles H. F.},

  abstractNote = {Cu/SSZ-13 Selective Catalytic Reduction (SCR) catalysts have been extensively studied for the past five-plus years. New and exciting fundamental and applied science has appeared in the literature quite frequently over this time. In this short review, a few topics specifically focused on a molecular-level understanding of this catalyst are summarized: (1) The nature of the active sites and, in particular, their transformations under varying reaction conditions that include dehydration, the presence of the various SCR reactants and hydrothermal aging; (2) Discussions of standard and fast SCR reaction mechanisms. Considerable progress has been made, especially in the last couple of years, on standard SCR mechanisms. In contrast, mechanisms for fast SCR are much less understood. Possible reaction paths are hypothesized for this latter case to stimulate further investigations; (3) Discussions of rational catalyst design based on new knowledge obtained regarding catalyst stability, overall catalytic performance and mechanistic catalytic chemistry.},

  doi          = {10.3390/catal8040140},

  journal      = {Catalysts},

  number       = 4,

  volume       = 8,

  place        = {United States},

  year         = {Sat Mar 31 00:00:00 EDT 2018},

  month        = {Sat Mar 31 00:00:00 EDT 2018}

}

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Title: Recent Progress in Atomic-Level Understanding of Cu/SSZ-13 Selective Catalytic Reduction Catalysts

Abstract

Citation Formats

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Nature of Cu Active Centers in Cu-SSZ-13 and Their Responses to SO 2 Exposure journal, January 2018

Interaction of NH 3 with Cu-SSZ-13 Catalyst: A Complementary FTIR, XANES, and XES Study journal, April 2014

Activity, propene poisoning resistance and hydrothermal stability of copper exchanged chabazite-like zeolite catalysts for SCR of NO with ammonia in comparison to Cu/ZSM-5 journal, June 2012

Integrated operando X-ray absorption and DFT characterization of Cu–SSZ-13 exchange sites during the selective catalytic reduction of NOx with NH3 journal, April 2012

The Cu-CHA deNO x Catalyst in Action: Temperature-Dependent NH 3 -Assisted Selective Catalytic Reduction Monitored by Operando XAS and XES journal, September 2016

The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites journal, February 2011

A comparison of hydrothermal aging effects on NH3-SCR of NO over Cu-SSZ-13 and Cu-SAPO-34 catalysts journal, April 2015

Understanding ammonia selective catalytic reduction kinetics over Cu/SSZ-13 from motion of the Cu ions journal, November 2014

Transformation of Active Sites in Fe/SSZ-13 SCR Catalysts during Hydrothermal Aging: A Spectroscopic, Microscopic, and Kinetics Study journal, March 2017

A comparative kinetics study between Cu/SSZ-13 and Fe/SSZ-13 SCR catalysts journal, December 2015

Sub-micron Cu/SSZ-13: Synthesis and application as selective catalytic reduction (SCR) catalysts journal, February 2017

Time-resolved copper speciation during selective catalytic reduction of NO on Cu-SSZ-13 journal, March 2018

Copper Coordination in Cu-SSZ-13 and Cu-SSZ-16 Investigated by Variable-Temperature XRD journal, December 2009

New insights into Cu/SSZ-13 SCR catalyst acidity. Part I: Nature of acidic sites probed by NH3 titration journal, April 2017

Catalysis in a Cage: Condition-Dependent Speciation and Dynamics of Exchanged Cu Cations in SSZ-13 Zeolites journal, April 2016

Effects of Si/Al ratio on Cu/SSZ-13 NH3-SCR catalysts: Implications for the active Cu species and the roles of Brønsted acidity journal, November 2015

NO oxidation: A probe reaction on Cu-SSZ-13 journal, April 2014

Atom-economical synthesis of a high silica CHA zeolite using a solvent-free route journal, January 2015

Isolation of the Copper Redox Steps in the Standard Selective Catalytic Reduction on Cu-SSZ-13 journal, September 2014

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 journal, May 2014

A comparative study of N2O formation during the selective catalytic reduction of NOx with NH3 on zeolite supported Cu catalysts journal, September 2015

The Dynamic Nature of Brønsted Acid Sites in Cu–Zeolites During NOx Selective Catalytic Reduction: Quantification by Gas-Phase Ammonia Titration journal, April 2015

Recent advances in the selective catalytic reduction of NOx with NH3 on Cu-Chabazite catalysts journal, March 2017

Influence of lattice stability on hydrothermal deactivation of Cu-ZSM-5 and Cu-IM-5 zeolites for selective catalytic reduction of NOx by NH3 journal, January 2014

Designed copper–amine complex as an efficient template for one-pot synthesis of Cu-SSZ-13 zeolite with excellent activity for selective catalytic reduction of NOx by NH3 journal, January 2011

Identification of two types of Cu sites in Cu/SSZ-13 and their unique responses to hydrothermal aging and sulfur poisoning journal, June 2016

Site-Specific Reactivity of Copper Chabazite Zeolites with Nitric Oxide, Ammonia, and Oxygen journal, November 2017

Reaction-driven Ion Exchange of Copper into Zeolite SSZ-13 journal, September 2015

High yield synthesis of high-silica chabazite by combining the role of zeolite precursors and tetraethylammonium: SCR of NOx journal, January 2015

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

Cu-exchanged Al-rich SSZ-13 zeolite from organotemplate-free synthesis as NH3-SCR catalyst: Effects of Na+ ions on the activity and hydrothermal stability journal, November 2017

The State of the Art in Selective Catalytic Reduction of NO x by Ammonia Using Metal‐Exchanged Zeolite Catalysts journal, December 2008

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

Current Understanding of Cu-Exchanged Chabazite Molecular Sieves for Use as Commercial Diesel Engine DeNOx Catalysts journal, August 2013

Composition-driven Cu-speciation and reducibility in Cu-CHA zeolite catalysts: a multivariate XAS/FTIR approach to complexity journal, January 2017

Dynamic multinuclear sites formed by mobilized copper ions in NO x selective catalytic reduction journal, August 2017

Hydrothermal stability of CuSSZ13 for reducing NOx by NH3 journal, March 2014

Coordination Environment of Copper Sites in Cu-CHA Zeolite Investigated by Electron Paramagnetic Resonance journal, September 2014

Two different cationic positions in Cu-SSZ-13? journal, January 2012

The role of pore size on the thermal stability of zeolite supported Cu SCR catalysts journal, August 2014

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

Location of Cu 2+ in CHA zeolite investigated by X-ray diffraction using the Rietveld/maximum entropy method journal, September 2014

Toward Rational Design of Cu/SSZ-13 Selective Catalytic Reduction Catalysts: Implications from Atomic-Level Understanding of Hydrothermal Stability journal, November 2017

Efficient One-Pot Preparation of Cu-SSZ-13 Materials using Cooperative OSDAs for their Catalytic Application in the SCR of NO x journal, May 2013

Redox-Driven Migration of Copper Ions in the Cu-CHA Zeolite as Shown by the In Situ PXRD/XANES Technique journal, July 2017

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

A Consistent Reaction Scheme for the Selective Catalytic Reduction of Nitrogen Oxides with Ammonia journal, March 2015

Experimental and Computational Interrogation of Fast SCR Mechanism and Active Sites on H-Form SSZ-13 journal, July 2017

Thermal durability of Cu-CHA NH3-SCR catalysts for diesel NOx reduction journal, April 2012

Effects of Alkali and Alkaline Earth Cocations on the Activity and Hydrothermal Stability of Cu/SSZ-13 NH 3 –SCR Catalysts journal, October 2015

Chemical deactivation of Cu-SSZ-13 ammonia selective catalytic reduction (NH3-SCR) systems journal, July 2014

Ammonia-Containing Species Formed in Cu-Chabazite As Per In Situ EPR, Solid-State NMR, and DFT Calculations journal, March 2015

Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts journal, November 2017

Effect of NO2 on the Selective Catalytic Reduction of NO with NH3 over Cu/SAPO-34 Molecular Sieve Catalyst journal, January 2014

Enhanced Performance for Selective Catalytic Reduction of NO x with NH 3 over Nanosized Cu/SAPO‐34 Catalysts journal, June 2019

Cu Loading Dependence of Fast NH3-SCR on Cu/SSZ-13 journal, March 2019

N–H bond activation in ammonia by TM-SSZ-13 (Fe, Co, Ni and Cu) zeolites: a first-principles calculation journal, January 2019

The dynamic nature of Cu sites in Cu-SSZ-13 and the origin of the seagull NO x conversion profile during NH 3 -SCR journal, January 2019

Temperature-dependent dynamics of NH 3 -derived Cu species in the Cu-CHA SCR catalyst journal, January 2019

Temperature-programmed reduction with NO as a characterization of active Cu in Cu-CHA catalysts for NH 3 -SCR journal, January 2019

Effects of SO 2 on Cu-SSZ-39 catalyst for the selective catalytic reduction of NO x with NH 3 journal, January 2020

Selective Catalytic Reduction of NOx journal, October 2018

The dynamic nature of Cu sites in Cu-SSZ-13 and the origin of the seagull NOx conversion profile during NH3-SCR null, January 2019

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

Nature of Cu Active Centers in Cu-SSZ-13 and Their Responses to SO ₂ Exposure
journal, January 2018

Interaction of NH ₃ with Cu-SSZ-13 Catalyst: A Complementary FTIR, XANES, and XES Study
journal, April 2014

Activity, propene poisoning resistance and hydrothermal stability of copper exchanged chabazite-like zeolite catalysts for SCR of NO with ammonia in comparison to Cu/ZSM-5
journal, June 2012

Integrated operando X-ray absorption and DFT characterization of Cu–SSZ-13 exchange sites during the selective catalytic reduction of NOx with NH3
journal, April 2012

The Cu-CHA deNO _x Catalyst in Action: Temperature-Dependent NH ₃ -Assisted Selective Catalytic Reduction Monitored by Operando XAS and XES
journal, September 2016

The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites
journal, February 2011

A comparison of hydrothermal aging effects on NH3-SCR of NO over Cu-SSZ-13 and Cu-SAPO-34 catalysts
journal, April 2015

Understanding ammonia selective catalytic reduction kinetics over Cu/SSZ-13 from motion of the Cu ions
journal, November 2014

Transformation of Active Sites in Fe/SSZ-13 SCR Catalysts during Hydrothermal Aging: A Spectroscopic, Microscopic, and Kinetics Study
journal, March 2017

A comparative kinetics study between Cu/SSZ-13 and Fe/SSZ-13 SCR catalysts
journal, December 2015

Sub-micron Cu/SSZ-13: Synthesis and application as selective catalytic reduction (SCR) catalysts
journal, February 2017

Time-resolved copper speciation during selective catalytic reduction of NO on Cu-SSZ-13
journal, March 2018

Copper Coordination in Cu-SSZ-13 and Cu-SSZ-16 Investigated by Variable-Temperature XRD
journal, December 2009

New insights into Cu/SSZ-13 SCR catalyst acidity. Part I: Nature of acidic sites probed by NH3 titration
journal, April 2017

Catalysis in a Cage: Condition-Dependent Speciation and Dynamics of Exchanged Cu Cations in SSZ-13 Zeolites
journal, April 2016

Effects of Si/Al ratio on Cu/SSZ-13 NH3-SCR catalysts: Implications for the active Cu species and the roles of Brønsted acidity
journal, November 2015

NO oxidation: A probe reaction on Cu-SSZ-13
journal, April 2014

Atom-economical synthesis of a high silica CHA zeolite using a solvent-free route
journal, January 2015

Isolation of the Copper Redox Steps in the Standard Selective Catalytic Reduction on Cu-SSZ-13
journal, September 2014

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
journal, May 2014

A comparative study of N2O formation during the selective catalytic reduction of NOx with NH3 on zeolite supported Cu catalysts
journal, September 2015

The Dynamic Nature of Brønsted Acid Sites in Cu–Zeolites During NOx Selective Catalytic Reduction: Quantification by Gas-Phase Ammonia Titration
journal, April 2015

Recent advances in the selective catalytic reduction of NOx with NH3 on Cu-Chabazite catalysts
journal, March 2017

Influence of lattice stability on hydrothermal deactivation of Cu-ZSM-5 and Cu-IM-5 zeolites for selective catalytic reduction of NOx by NH3
journal, January 2014

Designed copper–amine complex as an efficient template for one-pot synthesis of Cu-SSZ-13 zeolite with excellent activity for selective catalytic reduction of NOx by NH3
journal, January 2011

Identification of two types of Cu sites in Cu/SSZ-13 and their unique responses to hydrothermal aging and sulfur poisoning
journal, June 2016

Site-Specific Reactivity of Copper Chabazite Zeolites with Nitric Oxide, Ammonia, and Oxygen
journal, November 2017

Reaction-driven Ion Exchange of Copper into Zeolite SSZ-13
journal, September 2015

High yield synthesis of high-silica chabazite by combining the role of zeolite precursors and tetraethylammonium: SCR of NOx
journal, January 2015

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

Cu-exchanged Al-rich SSZ-13 zeolite from organotemplate-free synthesis as NH3-SCR catalyst: Effects of Na+ ions on the activity and hydrothermal stability
journal, November 2017

The State of the Art in Selective Catalytic Reduction of NO _x by Ammonia Using Metal‐Exchanged Zeolite Catalysts
journal, December 2008

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

Current Understanding of Cu-Exchanged Chabazite Molecular Sieves for Use as Commercial Diesel Engine DeNOx Catalysts
journal, August 2013

Composition-driven Cu-speciation and reducibility in Cu-CHA zeolite catalysts: a multivariate XAS/FTIR approach to complexity
journal, January 2017

Dynamic multinuclear sites formed by mobilized copper ions in NO _x selective catalytic reduction
journal, August 2017

Hydrothermal stability of CuSSZ13 for reducing NOx by NH3
journal, March 2014

Coordination Environment of Copper Sites in Cu-CHA Zeolite Investigated by Electron Paramagnetic Resonance
journal, September 2014

Two different cationic positions in Cu-SSZ-13?
journal, January 2012

The role of pore size on the thermal stability of zeolite supported Cu SCR catalysts
journal, August 2014

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

Location of Cu ²⁺ in CHA zeolite investigated by X-ray diffraction using the Rietveld/maximum entropy method
journal, September 2014

Toward Rational Design of Cu/SSZ-13 Selective Catalytic Reduction Catalysts: Implications from Atomic-Level Understanding of Hydrothermal Stability
journal, November 2017

Efficient One-Pot Preparation of Cu-SSZ-13 Materials using Cooperative OSDAs for their Catalytic Application in the SCR of NO _x
journal, May 2013

Redox-Driven Migration of Copper Ions in the Cu-CHA Zeolite as Shown by the In Situ PXRD/XANES Technique
journal, July 2017

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

A Consistent Reaction Scheme for the Selective Catalytic Reduction of Nitrogen Oxides with Ammonia
journal, March 2015

Experimental and Computational Interrogation of Fast SCR Mechanism and Active Sites on H-Form SSZ-13
journal, July 2017

Thermal durability of Cu-CHA NH3-SCR catalysts for diesel NOx reduction
journal, April 2012

Effects of Alkali and Alkaline Earth Cocations on the Activity and Hydrothermal Stability of Cu/SSZ-13 NH ₃ –SCR Catalysts
journal, October 2015

Chemical deactivation of Cu-SSZ-13 ammonia selective catalytic reduction (NH3-SCR) systems
journal, July 2014

Ammonia-Containing Species Formed in Cu-Chabazite As Per In Situ EPR, Solid-State NMR, and DFT Calculations
journal, March 2015

Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts
journal, November 2017

Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst
journal, January 2014

Enhanced Performance for Selective Catalytic Reduction of NO _x with NH ₃ over Nanosized Cu/SAPO‐34 Catalysts
journal, June 2019

Cu Loading Dependence of Fast NH3-SCR on Cu/SSZ-13
journal, March 2019

N–H bond activation in ammonia by TM-SSZ-13 (Fe, Co, Ni and Cu) zeolites: a first-principles calculation
journal, January 2019

The dynamic nature of Cu sites in Cu-SSZ-13 and the origin of the seagull NO _x conversion profile during NH ₃ -SCR
journal, January 2019

Temperature-dependent dynamics of NH ₃ -derived Cu species in the Cu-CHA SCR catalyst
journal, January 2019

Temperature-programmed reduction with NO as a characterization of active Cu in Cu-CHA catalysts for NH ₃ -SCR
journal, January 2019

Effects of SO ₂ on Cu-SSZ-39 catalyst for the selective catalytic reduction of NO _x with NH ₃
journal, January 2020

Selective Catalytic Reduction of NOx
journal, October 2018

The dynamic nature of Cu sites in Cu-SSZ-13 and the origin of the seagull NOx conversion profile during NH3-SCR
null, January 2019