Effective Local Geometry Descriptor for 29Si NMR Q4 Anisotropy

Venetos, Maxwell C.; Dwaraknath, Shyam; Persson, Kristin A.

doi:10.1021/acs.jpcc.1c04829

Title: Effective Local Geometry Descriptor for 29Si NMR Q4 Anisotropy

Journal Article · Thu Aug 26 00:00:00 EDT 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c04829· OSTI ID:1825012

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Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

The nuclear shielding anisotropy, ζ, is a useful nuclear magnetic resonance (NMR) shielding tensor parameter in describing the extent of electron cloud distortion about an atom. Despite the advantages afforded by NMR in structural characterization, the relationship between ζ and local structure of an atom in high-symmetry environments, such as Si-Q⁴ sites, is poorly understood. Here, we use a data-driven approach combining random forest feature ranking and the Sure Independence Screening and Sparsifying Operator (SISSO) approach to derive a simple and accurate geometric descriptor for ζ with a root-mean-squared prediction error of 6.77 ppm and an R² of 0.761. We then apply this descriptor to describe the local geometric distortion of zeolites Sigma-2 and silica-ZSM-5 whose chemical shift anisotropy tensor has been reported. We envision that this geometric descriptor will allow for structural description and refinement in previously difficult-to-describe materials.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES), Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1825012

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 35; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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