# Data sets for "Transformations to the aluminum coordination environment and network polymerization in amorphous aluminosilicates under pressure"

Data sets used to prepare Figures 1, 3-22, S1 and S3-S13 in the Journal of Chemical Physics article entitled "Transformations to the aluminum coordination environment and network polymerization in amorphous aluminosilicates under pressure." The data sets describe the structure of amorphous aluminosilicates under, or recovered from, high-pressure conditions. They were obtained by using in situ high-pressure neutron diffraction and solid-state 27Al nuclear magnetic resonance (NMR) spectrocopy. The results are discussed by reference to those obtained from in situ high-pressure x-ray diffraction and solid-state 17O, 27Al, 29Si NMR experiments.

Cite this dataset as:

Salmon, P.,
Zeidler, A.,
2024.
*Data sets for "Transformations to the aluminum coordination environment and network polymerization in amorphous aluminosilicates under pressure".*
Bath: University of Bath Research Data Archive.
Available from: https://doi.org/10.15125/BATH-01387.

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## Data

Fig1_27Al_NMR.agr

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Figure 1 shows the fitted ^{27}Al MAS NMR spectra for the CaAS_19_61 and CaAS_26_49 glasses recovered from high pressure conditions.

Fig4_Fofq_CaAS_26_49.agr

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Figure 4 shows the total structure factors F(k) measured using D4c for uncompressed, compressed or recovered CaAS_26_49 glass.

Fig5_k-space … positions.agr

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Figure 5 shows the pressure dependence of the FSDP position k_{FSDP} and principal peak position k_{PP} in the measured F(k) functions.

Fig6_EOS.agr

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Figure 6 shows the pressure-volume equation of state for calcium aluminosilicates.

Fig7_Dofr_CaAS1961_part1.agr

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Figure 7 shows the pressure dependence of several D'(r) functions for glassy CaAS_19_61.

Fig8_Dofr_CaAS2649_part1.agr

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Figure 8 shows the pressure dependence of several D'(r) functions for glassy CaAS_26_49.

Fig9_Dofr_CaAS_recovered.agr

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Figure 9 shows the fitted D'(r) functions for (a) and (b) glassy CaAS_19_61 and (c) glassy CaAS_26_49 recovered from high pressure conditions

Fig10_r-space_data.agr

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Figure 10 shows the pressure dependence of (a) the A-O bond distances (A = Si or Al) and (b) the Al-O coordination number.

Fig11_AlO_CN_vs_pmax.agr

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Figure 11 shows the dependence of the Al-O coordination number on the maximum applied pressure p_{max} in cold-compression experiments on glassy CaAS_26_49, CaAS_19_61, pyrope and MgAS_37.5_50.

Fig12_O-packing_v3.agr

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Figure 12 shows the dependence of the A-O coordination number for network-forming motifs (A = B, Ge, Si, or Si and Al) on the oxygen packing fraction for several glassy and liquid network-forming systems under pressure.

Fig16a_NBO … vs_model_v4.agr

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Figure 16(a) shows the measured versus calculated values of f_{NBO} for silicate and aluminosilicate glasses. The network formers were presumed to be all the Si(j) species and, in the case of the aluminosilicates, all the Al(j) species.

Fig16b_NBO … model_Al4+Al5.agr

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Figure 16(b) shows the measured versus calculated values of f_{NBO} for silicate and aluminosilicate glasses. The network formers were presumed to be all the Si(j) species and, in the case of the aluminosilicates, only the Al(IV) and Al(V) species.

Fig17a_fNBO … density_all_Al.agr

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Figure 17(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

Fig17b_fNBO … Al-O_CN_all_Al.agr

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Figure 17(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

Fig20a_fNBO … merised_Al4+Al5.agr

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Figure 20(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

Fig20b_fNBO … merised_Al4+Al5.agr

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Figure 20(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

Fig21_speciation_Drewitt_v3.agr

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Figure 21 shows the pressure dependence of the fractions of (a) Si(j) (j = IV, V or VI), (b) Al(j) (j = IV, V or VI), and (c) O-(Al,Si)_i (i = 1, 2, 3 or 4) species found from molecular dynamics simulations of hot-compressed CaAS_25_50 glass at 27 Celsius.

FigS1_27Al_NMR.agr

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Figure S1 shows the fitted ^{27}Al MAS NMR spectra for the uncompressed CaAS_19_61 and CaAS_26_49 glasses.

FigS3_Dofr_CaAS1961_part2.agr

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Figure S3 shows the pressure dependence of several D'(r) functions for glassy CaAS_19_61.

FigS4_Dofr_CaAS2649_part2.agr

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Figure S4 shows the pressure dependence of several D'(r) functions for glassy CaAS_26_49.

FigS5a_fNBO … depolymerised_Al4.agr

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Figure S5(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS5b_fNBO … depolymerised_Al4.agr

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Figure S5(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS7a_NBO … depolymerised_Al4.agr

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Figure S7(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS7b_NBO … depolymerised_Al4.agr

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Figure S7(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS9a_NBO … density_all_Al.agr

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Figure S9(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

FigS9b_NBO … Al-O_CN_all_Al.agr

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Figure S9(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

FigS12a_NBO … merised_Al4+Al5.jpg

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Figure S12(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

FigS12b_NBO … merised_Al4+Al5.agr

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Figure S12(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the depolymerized glasses with f_{NBO} ~0.22-0.24 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

Fig3_Fofq_CaAS_19_61_v2.agr

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Figure 3 shows the total structure factors F(k) measured using D4c for uncompressed, compressed or recovered CaAS_19_61 glass.

Fig13_Al-CN_vs_density_v8.agr

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Figure 13 shows Reduced density dependence of the Al-O coordination number for (a) calcium aluminosilicate glasses along or close to the tectosilicate tie-line and (b) a variety of other aluminosilicate glasses.

Fig14_Al_speciation … v2.agr

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Figure 14 shows the reduced density dependence of the aluminum speciation f_{Al(j)} found from ^{27}Al MAS NMR experiments on the uncompressed or recovered glasses of Fig. 13.

Fig15_Al-O … vs_density_v2.agr

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Figure 15 shows the reduced density dependence of the Al-O coordination number n_{Al}^{O} = 4f_{Al(IV)}+5f_{Al(V)}+6f_{Al(VI)} versus its contributions from the four- plus five-coordinated species, 4f_{Al(IV)}+5f_{Al(V)}, and from the six-coordinated species, 6f_{Al(VI)}.

Fig18a_fNBO … NBO_all_Al_v3.agr

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Figure 18(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

Fig18b_fNBO … NBO_all_Al_v3.agr

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Figure 18(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

Fig19a_fNBO … Al4+Al5_v2.agr

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Figure 19(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

Fig19b_fNBO … Al4+Al5_v2.agr

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Figure 19(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

FigS6a_fNBO … NBO_Al4_v2.agr

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Figure S6(a) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS6b_fNBO … NBO_Al4_v2.agr

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Figure S6(b) shows the dependence of the fraction of non-bridging oxygen atoms f_{NBO} on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS8a_NBO … polymerised_Al4_v3.agr

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Figure S8(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS8b_NBO … polymerised_Al4_v3.agr

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Figure S8(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV) and Al(IV) species contribute towards the network.

FigS10a_NBO … NBO_all_Al_v4.agr

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Figure S10(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

FigS10b_NBO … NBO_all_Al_v3.agr

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Figure S10(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and all the Si(IV) and aluminum species contribute towards the network.

FigS11a_NBO … Al4+Al5_v2.agr

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Figure S11(a) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the reduced density rho^prime for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

FigS11b_NBO … Al4+Al5_v2.agr

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Figure S11(b) shows the dependence of the number of non-bridging oxygen atoms per tetrahedron N_{NBO}/N_T on the Al-O coordination number for the tectosilicate glasses with f_{NBO} ~0 at rho^prime = 1. The fraction of NBO atoms was calculated by assuming that f_{Si(IV)} = 1 and only the Si(IV), Al(IV) and Al(V) species contribute towards the network.

Fig22_O2_vs_O3_density_v5.agr

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Figure 22 shows the reduced density dependence of the fractions of O(j) (j = I, II, III or IV) species for (a) glassy CaAS_25_50 at 27 Celsius, (b) liquid CaAS_25_50 at 2,227 Celsius, (c) glassy CaAS_19_61 and CaAS_26_49 at 25 Celsius, and (d) several recovered tectosilicate glasses.

FigS13_O2_vs_O3_v3.agr

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Figure S13 shows the pressure dependence of the fractions of O(j) (j = I, II, III or IV) species for (a) glassy CaAS_25_50 at 27 Celsius, (b) liquid CaAS_25_50 at 2,227 Celsius, and (c) glassy CaAS_19_61 and CaAS_26_49 at 25 Celsius.

## Coverage

Collection date(s):

From 9 May 2018 to 14 June 2024

## Documentation

Data collection method:

The data sets were collected using the methods described in the published paper.

Data processing and preparation activities:

The data sets were analysed using the methods described in the published paper.

Technical details and requirements:

The figures were prepared using QtGrace (https://sourceforge.net/projects/qtgrace/). The data set corresponding to a plotted curve within an QtGrace file can be identified by clicking on that curve.

Additional information:

The files are labelled according to the corresponding figure numbers. The units for each axis are identified on the plots.

## Funders

Engineering and Physical Sciences Research Council

https://doi.org/10.13039/501100000266

EPSRC Centre for Doctoral Training in Condensed Matter Physics

EP/L015544/1

Royal Society

https://doi.org/10.13039/501100000288

Dorothy Hodgkin Research Fellowship - Rational Design of Glassy Materials with Technological Applications

DH140152

Diamond Light Source

https://doi.org/10.13039/100011889

ISIS/Diamond Facility Development Studentship

STU0173

ISIS Neutron and Muon Source (The ISIS Neutron and Muon Source)

https://doi.org/10.13039/501100021200

ISIS/Diamond Facility Development Studentship

STU0173

## Publication details

Publication date: 6 August 2024

by: University of Bath

Version: 1

DOI: https://doi.org/10.15125/BATH-01387

URL for this record: https://researchdata.bath.ac.uk/id/eprint/1387

## Related papers and books

Gammond, L. V. D., Zeidler, A., Youngman, R. E., Fischer, H. E., Bull, C. L., and Salmon, P. S.,
2024.
Transformations to the aluminum coordination environment and network polymerization in amorphous aluminosilicates under pressure.
*The Journal of Chemical Physics*, 161(7).
Available from: https://doi.org/10.1063/5.0218574.

## Contact information

Please contact the Research Data Service in the first instance for all matters concerning this item.

Contact person: Philip Salmon

Faculty of Science

Physics

Research Centres & Institutes

Centre for Nanoscience and Nanotechnology