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Achieving Atomic Dispersion of Highly Loaded Transition Metals in Small-Pore Zeolite SSZ-13: High-Capacity and High-Efficiency Low-Temperature CO and Passive NOx Adsorbers

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [1];  [3];  [4];  [4];  [4];  [5];  [5];  [5];  [2];  [1];  [1]
  1. Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland WA 99352 USA
  2. 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
  3. Chemistry Department, Brookhaven National Laboratory, Uptown NY 11973 USA
  4. Department of Chemical and Petroleum Engineering and Center for Environmentally Beneficial Catalysis, University of Kansas, Lawrence KS 66045 USA
  5. Faculty of Chemistry and Pharmacy, University of Sofia, 1126 Sofia Bulgaria
+ Show Author Affiliations

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 a combined spectroscopic and DFT approach, we offer a unifying explana-tion for the discrepancies existing in available M-zeolite litera-ture. Moreover, we highlight the difference between the behavior of Pt and Pd during synthesis, and demonstrate that ionically dispersed Pd/SSZ-13 shows superior performance as a new class of environmentally important passive NOx Adsorber (PNA) material under practically relevant conditions. It thus represents the 2nd known metal-small pore zeolite material that has immediate industrial application, and the only known met-al-small pore zeolite material in which metal is close to 100 % utilized. In addition to NOx, the material performs remarkably for CO removal during cold start as well due to the formation of a mixed carbonyl-nitrosyl complex Pd(II)(CO)(NO).

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1490338
Report Number(s):
PNNL-SA-136340
Journal Information:
Angewandte Chemie (International Edition), Vol. 57, Issue 51; ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English

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