TY - JOUR
T1 - Coke Formation in a Zeolite Crystal During the Methanol-to- Hydrocarbons Reaction as Studied with Atom Probe Tomography
AU - Schmidt, Joel E
AU - Poplawsky, Jonathan D
AU - Mazumder, Baishakhi
AU - Attila, Özgün
AU - Fu, Donglong
AU - Winter, D A Matthijs De
AU - Meirer, Florian
AU - Bare, Simon R
AU - Weckhuysen, Bert M
PY - 2016
Y1 - 2016
N2 - Understanding the formation of carbon deposits in zeolites is vital to developing new,superior materials for various applications,including oil and gas conversion pro- cesses.Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub- nm length scale in asingle zeolite ZSM-5 crystal, whichhas been partially deactivated by the methanol-to-hydrocarbons reaction using 13 C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters withamedian size of 30– 60 13 Catoms.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. This nanoscale correlation underscores the importance of carefully engineer- ing materials to suppress detrimental coke formation.
AB - Understanding the formation of carbon deposits in zeolites is vital to developing new,superior materials for various applications,including oil and gas conversion pro- cesses.Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub- nm length scale in asingle zeolite ZSM-5 crystal, whichhas been partially deactivated by the methanol-to-hydrocarbons reaction using 13 C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters withamedian size of 30– 60 13 Catoms.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. This nanoscale correlation underscores the importance of carefully engineer- ing materials to suppress detrimental coke formation.
U2 - 10.1002/anie.201606099
DO - 10.1002/anie.201606099
M3 - Article
SN - 1433-7851
VL - 55
SP - 11173
EP - 11177
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
ER -