4.8 Article

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

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 51, Pages 16672-16677

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201809343

Keywords

CO adsorber; NOx; palladium; platinum; zeolites

Funding

  1. U.S. Department of Energy (DOE),Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program
  2. DOE's Office of Biological and Environmental Research
  3. Bulgarian Science Fund [DFNI-T02/20]
  4. European Regional Development Fund
  5. Operational Program Science and Education for Smart Growth under contract UNITe [BG05M2OP001-1.001-0004-C01]
  6. Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-SC0014561]
  7. National Science Foundation [NSF-OIA-1539105]

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The majority of harmful atmospheric CO and NOx emissions are from vehicle exhausts. Although there has been success addressing NOx emissions at temperatures above 250 degrees C with selective catalytic reduction technology, emissions during vehicle cold start (when the temperature is below 150 degrees C), are a major challenge. Herein, we show we can completely eliminate both CO and NOx emissions simultaneously under realistic exhaust flow, using a highly loaded (2wt%) atomically dispersed palladium in the extra-framework positions of the small-pore chabazite material as a CO and passive NOx adsorber. Until now, atomically dispersed highly loaded (>0.3wt%) transition-metal/SSZ-13 materials have not been known. We devised a general, simple, and scalable route to prepare such materials for Pt-II and Pd-II. Through spectroscopy and materials testing we show that both CO and NOx can be simultaneously completely abated with 100% efficiency by the formation of mixed carbonyl-nitrosyl palladium complex in chabazite micropore.

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