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Title: Quasi-operando quantification of Cu(ii) ions in Cu-SSZ-13 catalyst by an NH3 temperature-programmed reduction method

Journal Article · · ChemComm
DOI: https://doi.org/10.1039/d0cc07346f · OSTI ID:1778839
 [1]; ORCiD logo [2];  [2];  [2];  [2];  [3];  [2]; ORCiD logo [2]; ORCiD logo [4];  [2]
  1. Tsinghua Univ., Beijing (China). Key Laboratory of Advanced Materials of Ministry of Education, School of Materials Science and Engineering; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
  2. Tsinghua Univ., Beijing (China). Key Laboratory of Advanced Materials of Ministry of Education, School of Materials Science and Engineering
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
+ Show Author Affiliations

In this work, a quasi-operando NH3 temperature-programmed reduction method (NH3-TPR), with N2:Cu = 1:1, is developed to quantify total Cu(II) ions in Cu-SSZ-13 quenched from SCR-relevant reactions, and its accuracy is confirmed by in situ EPR. [Cu(OH)]+-Z and Cu2+-2Z can be further distinguished by NH3 reduction temperatures, and their different reducibility in SCR is revealed.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
National Key Research and Development Program of China; Tsinghua Scholarship for Overseas Graduate Studies; USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1778839
Report Number(s):
PNNL--SA-157387
Journal Information:
ChemComm, Journal Name: ChemComm Journal Issue: 15 Vol. 57; ISSN 1359-7345
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (17)

Isolation of the Copper Redox Steps in the Standard Selective Catalytic Reduction on Cu-SSZ-13 journal September 2014
Site-Specific Reactivity of Copper Chabazite Zeolites with Nitric Oxide, Ammonia, and Oxygen journal November 2017
In Situ Spectroscopic Studies on the Redox Cycle of NH 3 −SCR over Cu−CHA Zeolites journal April 2020
The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites journal February 2011
Quantitative analysis of active oxygen for soot oxidation over Ag/ZrO2: Characterization with temperature-programmed reduction by NH3 journal July 2012
In-situ studies of oxidation/reduction of copper in Cu-CHA SCR catalysts: Comparison of fresh and SO2-poisoned catalysts journal July 2020
Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3 journal October 2010
Effects of NO 2 Addition on the NH 3 -SCR over Small-Pore Cu–SSZ-13 Zeolites with Varying Cu Loadings journal October 2018
Ammonia-Containing Species Formed in Cu-Chabazite As Per In Situ EPR, Solid-State NMR, and DFT Calculations journal March 2015
Probing Active-Site Relocation in Cu/SSZ-13 SCR Catalysts during Hydrothermal Aging by In Situ EPR Spectroscopy, Kinetics Studies, and DFT Calculations journal June 2020
Toward Rational Design of Cu/SSZ-13 Selective Catalytic Reduction Catalysts: Implications from Atomic-Level Understanding of Hydrothermal Stability journal November 2017
Nature of Cu Active Centers in Cu-SSZ-13 and Their Responses to SO 2 Exposure journal January 2018
Speciation of Cu Cations in Cu-CHA Catalysts for NH 3 -SCR: Effects of SiO 2 /AlO 3 Ratio and Cu-Loading Investigated by Transient Response Methods journal August 2019
Catalysis in a Cage: Condition-Dependent Speciation and Dynamics of Exchanged Cu Cations in SSZ-13 Zeolites journal April 2016
Interaction of NH 3 with Cu-SSZ-13 Catalyst: A Complementary FTIR, XANES, and XES Study journal April 2014
Detection of key transient Cu intermediates in SSZ-13 during NH 3 -SCR deNO x by modulation excitation IR spectroscopy journal January 2020
Dynamic multinuclear sites formed by mobilized copper ions in NO x selective catalytic reduction journal August 2017

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