A quantitative study of the structure–activity relationship in hierarchical zeolites using liquid-phase reactions

Dandan Xu, Omar Abdelrahman, Sang Hyun Ahn, Yasmine Guefrachi, Anatoliy Kuznetsov, Limin Ren, Sonjong Hwang, Maryam Khaleel, Saeed Al Hassan, Dongxia Liu, Suk Bong Hong, Paul J Dauenhauer, Michael Tsapatsis

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

Micro/meso/macroporous (hierarchical) zeolites show remarkable catalytic performance for reactions involving bulky reactants. However, quantitative assessment of the microstructural characteristics contributing to the observed performance remains elusive. Here, structure–activity relationships are established for a set of micro/mesoporous self-pillared pentasil (SPP) zeolites using two parallel liquid-phase reactions (benzyl alcohol alkylation and self-etherification) based on analysis of mass transport and reaction kinetics. A reaction–diffusion mathematical model is developed that quantitatively assigns the catalytic contributions of the external surface and micropores of SPP zeolites for these reactions. In addition, the effect of the zeolite external surface structure on the corresponding catalytic activity is quantitatively assessed by comparing SPP zeolites (with MFI structure) with MCM-22 (with MWW structure). This work demonstrates that reaction–diffusion modeling allows quantitative description of the catalytic performance of hierarchical zeolites and provides a model reaction to assess nm-sized characteristic diffusion lengths in MFI.

Original languageEnglish (US)
Pages (from-to)1067-1075
Number of pages9
JournalAIChE Journal
Volume65
Issue number3
DOIs
StatePublished - Mar 1 2019

Fingerprint

Zeolites
Liquids
Benzyl Alcohol
Alkylation
Multicarrier modulation
Reaction kinetics
Surface structure
Catalyst activity
Alcohols
Mass transfer
Mathematical models
Theoretical Models

Keywords

  • hierarchical zeolites
  • kinetics
  • liquid-phase alkylation and etherification
  • reaction–diffusion modeling
  • surface topology

Cite this

A quantitative study of the structure–activity relationship in hierarchical zeolites using liquid-phase reactions. / Xu, Dandan; Abdelrahman, Omar; Ahn, Sang Hyun; Guefrachi, Yasmine; Kuznetsov, Anatoliy; Ren, Limin; Hwang, Sonjong; Khaleel, Maryam; Al Hassan, Saeed; Liu, Dongxia; Hong, Suk Bong; Dauenhauer, Paul J; Tsapatsis, Michael.

In: AIChE Journal, Vol. 65, No. 3, 01.03.2019, p. 1067-1075.

Research output: Contribution to journalArticle

Xu, D, Abdelrahman, O, Ahn, SH, Guefrachi, Y, Kuznetsov, A, Ren, L, Hwang, S, Khaleel, M, Al Hassan, S, Liu, D, Hong, SB, Dauenhauer, PJ & Tsapatsis, M 2019, 'A quantitative study of the structure–activity relationship in hierarchical zeolites using liquid-phase reactions', AIChE Journal, vol. 65, no. 3, pp. 1067-1075. https://doi.org/10.1002/aic.16503
Xu, Dandan ; Abdelrahman, Omar ; Ahn, Sang Hyun ; Guefrachi, Yasmine ; Kuznetsov, Anatoliy ; Ren, Limin ; Hwang, Sonjong ; Khaleel, Maryam ; Al Hassan, Saeed ; Liu, Dongxia ; Hong, Suk Bong ; Dauenhauer, Paul J ; Tsapatsis, Michael. / A quantitative study of the structure–activity relationship in hierarchical zeolites using liquid-phase reactions. In: AIChE Journal. 2019 ; Vol. 65, No. 3. pp. 1067-1075.
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