Brønsted acidity in zeolites measured by deprotonation energy
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F22%3A00557524" target="_blank" >RIV/61388963:_____/22:00557524 - isvavai.cz</a>
Alternative codes found
RIV/00216275:25310/22:39919518
Result on the web
<a href="https://doi.org/10.1038/s41598-022-11354-x" target="_blank" >https://doi.org/10.1038/s41598-022-11354-x</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1038/s41598-022-11354-x" target="_blank" >10.1038/s41598-022-11354-x</a>
Alternative languages
Result language
angličtina
Original language name
Brønsted acidity in zeolites measured by deprotonation energy
Original language description
Acid forms of zeolites have been used in industry for several decades but scaling the strength of their acid centers is still an unresolved and intensely debated issue. In this paper, the Bronsted acidity strength in aluminosilicates measured by their deprotonation energy (DPE) was investigated for FAU, CHA, IFR, MOR, FER, MFI, and TON zeolites by means of periodic and cluster calculations at the density functional theory (DFT) level. The main drawback of the periodic DFT is that it does not provide reliable absolute values due to spurious errors associated with the background charge introduced in anion energy calculations. To alleviate this problem, we employed a novel approach to cluster generation to obtain accurate values of DPE. The cluster models up to 150 T atoms for the most stable Bronsted acid sites were constructed on spheres of increasing diameter as an extension of Harrison's approach to calculating Madelung constants. The averaging of DPE for clusters generated this way provides a robust estimate of DPE for investigated zeolites despite slow convergence with the cluster size. The accuracy of the cluster approach was further improved by a scaled electrostatic embedding scheme proposed in this work. The electrostatic embedding model yields the most reliable values with the average deprotonation energy of about 1245 +/- 9 kJ center dot mol(-1) for investigated acidic zeolites. The cluster calculations strongly indicate a correlation between the deprotonation energy and the zeolite framework density. The DPE results obtained with our electrostatic embedding model are highly consistent with the previously reported QM/MM and periodic calculations.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
—
OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
<a href="/en/project/GA19-19542S" target="_blank" >GA19-19542S: A Structure-Based Predictive Model for Brønsted Acid Catalyzed Reactions</a><br>
Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2022
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Scientific Reports
ISSN
2045-2322
e-ISSN
2045-2322
Volume of the periodical
12
Issue of the periodical within the volume
1
Country of publishing house
GB - UNITED KINGDOM
Number of pages
9
Pages from-to
7301
UT code for WoS article
000790941900036
EID of the result in the Scopus database
2-s2.0-85129429595