2018
DOI: 10.1021/acs.jpcc.8b08684
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On the Rational Design of Zeolite Clusters for Converging Reaction Barriers: Quantum Study of Aldol Kinetics Confined in HZSM-5

Abstract: We have performed density functional theory calculations to investigate the convergence of reaction barriers with respect to zeolite cluster size, for multistep reactions catalyzed in HZSM-5. We constructed cluster models of HZSM-5 using the delta-cluster approach reported previously by us. We then computed barriers for different reaction types to determine the cluster sizes and neighbor-list radii needed to fully treat zeolite confinement effects. In particular, we studied the acid-zeolite-catalyzed aldol rea… Show more

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Cited by 8 publications
(6 citation statements)
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“…Then, in a second step, the hydrogen atoms at the cluster boundaries were frozen, and the other atoms were optimized. The clusters have typically over 50 T atoms, which are of comparable size as previously reported to reach convergence of reaction barriers in catalytic reactions of zeolites …”
Section: Resultsmentioning
confidence: 55%
See 1 more Smart Citation
“…Then, in a second step, the hydrogen atoms at the cluster boundaries were frozen, and the other atoms were optimized. The clusters have typically over 50 T atoms, which are of comparable size as previously reported to reach convergence of reaction barriers in catalytic reactions of zeolites …”
Section: Resultsmentioning
confidence: 55%
“…The clusters have typically over 50 T atoms, which are of comparable size as previously reported to reach convergence of reaction barriers in catalytic reactions of zeolites. 84 It is an important prerequisite for the successful calculation of 27 Al chemical shifts that the local structure at the central Al atom be described as realistically as possible. This is particularly important as the Al−O−Si bond angles are highly relevant for the 27 Al chemical shifts (see above).…”
Section: Resultsmentioning
confidence: 99%
“…On the one hand, cluster studies are relatively simple and can be applied to a wide range of structures. For instance, Migues et al [34,35] developed a systematic method to construct cluster models that ensure the convergence of the energetic effects of the selected zeolite-catalyzed reactions. On the other hand, cluster calculations may miss some information on the long-range interactions within the bulk, which are otherwise captured by periodic calculations.…”
Section: Resultsmentioning
confidence: 99%
“…Unfortunately, the mechanism for HMF formation from LGO remains unknown at present, which may restrict the optimization of HMF production from LGO. Herein, this study tends to clarify the mechanism for HMF formation from LGO or DH without and with sulfuric acid-catalyzed hydrolysis using density functional theory (DFT) calculations employing the B3LYP method, which has been widely used in mechanistic studies, especially for the cellulose-derived chemicals. …”
Section: Introductionmentioning
confidence: 99%