Spectroscopic Signatures of Internal Hydrogen Bonds of Bronsted-Acid Sites in the Zeolite H-MFI

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F23%3A10471051" target="_blank" >RIV/00216208:11310/23:10471051 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=fcTNKVxnF7" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=fcTNKVxnF7</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/anie.202303204" target="_blank" >10.1002/anie.202303204</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Spectroscopic Signatures of Internal Hydrogen Bonds of Bronsted-Acid Sites in the Zeolite H-MFI

Popis výsledku v původním jazyce

The location of Brønsted-acid sites (bridging OH groups, b-OH) at different crystallographic positions of zeolite catalysts influences their reactivity due to varying confinement. Selecting the most stable b-OH conformers at each of the 12 T-sites (T=Si/Al) of H-MFI, a representative set of 26 conformers is obtained which includes free b-OH groups pointing into the empty pore space and b-OH groups forming H-bonds across five- or six-membered rings of TO4 tetrahedra. Chemically accurate coupled-cluster-quality calculations for periodic models show that the strength of internal H-bonds and, hence, the OH bond length vary substantially with the framework position. For 11 of the 19 H-bonded b-OH groups examined, our predictions fall into the full width at half maximum range of the experimental signals at 3250 +/- 175 cm(-1) and 7.0 +/- 1.4 ppm which supports previously debated assignments of these signals to H-bonded b-OH sites.

Název v anglickém jazyce

Spectroscopic Signatures of Internal Hydrogen Bonds of Bronsted-Acid Sites in the Zeolite H-MFI

Popis výsledku anglicky

The location of Brønsted-acid sites (bridging OH groups, b-OH) at different crystallographic positions of zeolite catalysts influences their reactivity due to varying confinement. Selecting the most stable b-OH conformers at each of the 12 T-sites (T=Si/Al) of H-MFI, a representative set of 26 conformers is obtained which includes free b-OH groups pointing into the empty pore space and b-OH groups forming H-bonds across five- or six-membered rings of TO4 tetrahedra. Chemically accurate coupled-cluster-quality calculations for periodic models show that the strength of internal H-bonds and, hence, the OH bond length vary substantially with the framework position. For 11 of the 19 H-bonded b-OH groups examined, our predictions fall into the full width at half maximum range of the experimental signals at 3250 +/- 175 cm(-1) and 7.0 +/- 1.4 ppm which supports previously debated assignments of these signals to H-bonded b-OH sites.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/EF15_003%2F0000417" target="_blank" >EF15_003/0000417: Centrum pro cílenou syntézu a aplikace perspektivních materiálů</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

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

Název periodika

Angewandte Chemie - International Edition

ISSN

1433-7851

e-ISSN

1521-3773

Svazek periodika

62

Číslo periodika v rámci svazku

25

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

5

Strana od-do

e202303204

Kód UT WoS článku

000985847700001

EID výsledku v databázi Scopus

2-s2.0-85158879547