Thermodynamic driving forces for autoreduction of Cu sites in the zeolite SSZ-13

Daniel J. Hutton, David H. Lopez, Florian Göltl

Research output: Contribution to journalArticlepeer-review

Abstract

Cu-exchanged zeolites are widely used redox catalysts and the oxidation state of Cu is crucial in understanding their performance over a wide range of applications. Interestingly, a fraction of Cu sites in zeolites is reported to reduce at high temperatures in the absence of a reducing agent and as of today a detailed understanding of this process is still missing. In this contribution, we use first principles-based phase diagrams to explore thermodynamic driving forces for the autoreduction of Cu sites in the zeolite SSZ-13. We find that mainly monovalent Cu(ii)-OH sites anchored at well-separated Al atoms and to a lesser degree di-hydroxyl Cu dimers drive the autoreduction of Cu sites in the zeolite SSZ-13. Using these insights, we can reproduce experimental trends in autoreduction reported in the literature. This work gives detailed insights into the autoreduction of Cu sites in SSZ-13 and demonstrates that the nature of Cu sites in the zeolite SSZ-13 depends on the exact conditions the material is exposed to. Optimizing these reaction conditions might allow to improve the performance of Cu-exchanged zeolites over a wide range of applications.

Original languageEnglish (US)
JournalReaction Chemistry and Engineering
DOIs
StateAccepted/In press - 2024

ASJC Scopus subject areas

  • Catalysis
  • Chemistry (miscellaneous)
  • Chemical Engineering (miscellaneous)
  • Process Chemistry and Technology
  • Fluid Flow and Transfer Processes

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