Isoreticular UTL-Derived Zeolites as Model Materials for Probing Pore Size-Activity Relationship

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F19%3A10403409" target="_blank" >RIV/00216208:11310/19:10403409 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=S3NijiG6W1" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=S3NijiG6W1</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.9b00950" target="_blank" >10.1021/acscatal.9b00950</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Isoreticular UTL-Derived Zeolites as Model Materials for Probing Pore Size-Activity Relationship

Popis výsledku v původním jazyce

The relationship between the chemical composition and the activity of zeolites has been unambiguously established and used to optimize some reactions. However, the relationship between the micropore size and the activity of catalysts remains elusive. Here, we report the combination of the ADOR approach and postsynthetic alumination for the preparation of isoreticular Al-IPC materials as model catalysts to assess the effect of micropore size on their catalytic activity. XRD, SEM, N-2 ad-/desorption, chemical analysis, Al-27 NMR, and FTIR spectroscopy of adsorbed acetonitrile-d(3) show that the prepared isoreticular Al-IPC zeolites have similar Al content and coordination states as well as similar types and total numbers of acid sites but differ in micropore size, decreasing in the following order: Al-IPC-7 (14, 12, and 10-ring channels) &gt; Al-IPC-2 (12 and 10) &gt; Al-IPC-6 (12, 10, and 8) &gt; Al-IPC-4 (10 and 8). Furthermore, the kinetic study of gas-phase ethanol-to diethyl ether transformation evidenced a lack of confinement in ethanol dimers of IPC-6 and IPC-4 (k(first) = 0.4-0.9 mol(DEE) (mol(H+).s)(-1)) compared with IPC-2 (k(first) = 3.8 mol(DEE) (mol(H+).s)(-1)) and IPC-7 (k(first) = 6.3 mol(DEE) (mol(H+).s)(-1)) zeolites. The catalytic activity of IPC-zeolites in liquid-phase tetrahydropyranylation was correlated with the relative concentration of acid sites on the external surface of Al-IPC-n crystals, both increasing in the following order: IPC-4 (35% of &quot;external&quot; acid sites) &lt; IPC-6 (29%) &lt; IPC-2 (25%) &lt; IPC-7 (21%). The use of Al-IPC-n as model catalysts in important acid-catalyzed reactions can shed a light on the fundamental structure-activity relationship and help to improve or optimize existing catalytic processes.

Název v anglickém jazyce

Isoreticular UTL-Derived Zeolites as Model Materials for Probing Pore Size-Activity Relationship

Popis výsledku anglicky

The relationship between the chemical composition and the activity of zeolites has been unambiguously established and used to optimize some reactions. However, the relationship between the micropore size and the activity of catalysts remains elusive. Here, we report the combination of the ADOR approach and postsynthetic alumination for the preparation of isoreticular Al-IPC materials as model catalysts to assess the effect of micropore size on their catalytic activity. XRD, SEM, N-2 ad-/desorption, chemical analysis, Al-27 NMR, and FTIR spectroscopy of adsorbed acetonitrile-d(3) show that the prepared isoreticular Al-IPC zeolites have similar Al content and coordination states as well as similar types and total numbers of acid sites but differ in micropore size, decreasing in the following order: Al-IPC-7 (14, 12, and 10-ring channels) &gt; Al-IPC-2 (12 and 10) &gt; Al-IPC-6 (12, 10, and 8) &gt; Al-IPC-4 (10 and 8). Furthermore, the kinetic study of gas-phase ethanol-to diethyl ether transformation evidenced a lack of confinement in ethanol dimers of IPC-6 and IPC-4 (k(first) = 0.4-0.9 mol(DEE) (mol(H+).s)(-1)) compared with IPC-2 (k(first) = 3.8 mol(DEE) (mol(H+).s)(-1)) and IPC-7 (k(first) = 6.3 mol(DEE) (mol(H+).s)(-1)) zeolites. The catalytic activity of IPC-zeolites in liquid-phase tetrahydropyranylation was correlated with the relative concentration of acid sites on the external surface of Al-IPC-n crystals, both increasing in the following order: IPC-4 (35% of &quot;external&quot; acid sites) &lt; IPC-6 (29%) &lt; IPC-2 (25%) &lt; IPC-7 (21%). The use of Al-IPC-n as model catalysts in important acid-catalyzed reactions can shed a light on the fundamental structure-activity relationship and help to improve or optimize existing catalytic processes.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

Návaznosti

S - Specificky vyzkum na vysokych skolach<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2019

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ACS Catalysis

ISSN

2155-5435

e-ISSN

—

Svazek periodika

9

Číslo periodika v rámci svazku

6

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

11

Strana od-do

5136-5146

Kód UT WoS článku

000471212600041

EID výsledku v databázi Scopus

2-s2.0-85067115671