Cooperativity of silanol defect chemistry in zeolites

Literature Information

Publication Date 2022-12-01
DOI 10.1039/D2CP05218K
Impact Factor 3.676
Authors

Ya-Fan Chen, Christian Schroeder, Christopher M. Lew, Stacey I. Zones, Hubert Koller, Marek Sierka


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Abstract

Deboronation treatment of zeolite B-SSZ-55 can generate vacancy defects consisting of four silanol groups (silanol nests). However, 1H solid-state NMR spectroscopy indicates the prevalence of two silanol groups (silanol dyads) instead of four silanol groups. Such silanol dyads must be formed by the silanol condensation of two silanol groups at the silanol nests. Yet, the exact mechanism of this condensation and detailed structure of the silanol defect are not known. Here, the structure and formation mechanism of silanol dyads in the SSZ-55 zeolite have been investigated by both cluster and periodic density functional theory calculations. The calculated 1H NMR chemical shifts agree with the experimental values, showing that the silanol dyads are indeed commonly present at the vacancies and the vacancy density plays a role in the relaxation of the zeolite framework. The nature (size) of the silanol clusters influences their acidity.

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Contents list

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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