Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography
- Utrecht Univ., Utrecht (Netherlands)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
Understanding the formation of carbon deposits in zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub-nm length scale in a single zeolite ZSM-5 crystal, which has been partially deactivated by the methanol-to-hydrocarbons reaction using 13C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters with a median size of 30–60 13C atoms. These clusters correlate with local increases in Brønsted acid site density, demonstrating that the formation of the first deactivating coke precursor molecules occurs in nanoscopic regions enriched in aluminum. Here, this nanoscale correlation underscores the importance of carefully engineering materials to suppress detrimental coke formation.
- Research Organization:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- Grant/Contract Number:
- AC05-00OR22725
- OSTI ID:
- 1324189
- Journal Information:
- Angewandte Chemie (International Edition), Vol. 55, Issue 37; ISSN 1433-7851
- Publisher:
- WileyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Similar Records
Detecting Cage Crossing and Filling Clusters of Magnesium and Carbon Atoms in Zeolite SSZ-13 with Atom Probe Tomography
Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts