The Role of Water Loading and Germanium Content in Germanosilicate Hydrolysis
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F21%3A10436085" target="_blank" >RIV/00216208:11310/21:10436085 - isvavai.cz</a>
Result on the web
<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=Ihl.rJm9ZD" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=Ihl.rJm9ZD</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.jpcc.1c06873" target="_blank" >10.1021/acs.jpcc.1c06873</a>
Alternative languages
Result language
angličtina
Original language name
The Role of Water Loading and Germanium Content in Germanosilicate Hydrolysis
Original language description
The Assembly-Disassembly-Organization-Reassembly (ADOR) process has been used extensively to prepare new zeolite frameworks based on germanosilicate precursors. The disassembly step exploits the lability of the bonds in the presence of water to selectively disconnect the framework, prior to reorganization into new framework topologies. However, a mechanistic understanding of this crucial step is lacking: specifically, the roles of heteroatom (germanium) content and water loading in zeolite hydrolytic instability. In this work, ab initio free energy simulations, coupled with water vapor adsorption measurements reveal that collectivity effects control the reactivity of the archetypal ADORable zeolite UTL toward water. A transition between reversible and irreversible water adsorption occurs as water loading is increased, leading to reactive transformations. Clustering of germanium is observed to activate hitherto unreported favorable hydrolysis mechanisms beyond a threshold concentration of three atoms per double four ring unit, demonstrating that the heteroatom distribution and collectivity in the hydrolysis mechanism can drastically influence zeolite framework instability. These findings suggest that control over heteroatom content, distribution, and hydration level is important to achieve the controlled partial hydrolysis of zeolitic frameworks and is likely to apply not only to other ADORable germanosilicate zeolites but also to Lewis acidic zeolites in general.
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
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OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
Result was created during the realization of more than one project. More information in the Projects tab.
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2021
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Journal of Physical Chemistry C
ISSN
1932-7447
e-ISSN
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Volume of the periodical
125
Issue of the periodical within the volume
43
Country of publishing house
US - UNITED STATES
Number of pages
14
Pages from-to
23744-23757
UT code for WoS article
000716453300018
EID of the result in the Scopus database
2-s2.0-85118921002