Understanding hydrogen bonding in calcium silicate hydrate combining solid-state NMR and first principle calculations

Bo Li; Neng Li; H.J.H. Brouwers; Qingliang Yu; Wei Chen

doi:10.1016/j.conbuildmat.2019.117347

Understanding hydrogen bonding in calcium silicate hydrate combining solid-state NMR and first principle calculations

Bo Li, Neng Li, H.J.H. Brouwers, Qingliang Yu, Wei Chen (Corresponding author)

Building Materials

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

Mechanisms of hydrogen bonding and molecular structure in the C-S-H are investigated by combining results of ²⁹Si, ¹H solid SSNMR analysis and first principle calculations. First principle calculations for ¹H chemical shifts are used to correlate the observed ¹H SSNMR spectra with the underlying structure of various hydrogen bonds between different silicon moieties and hydrogen groups in the C-S-H gels. The results show that strong hydrogen bonds are formed between water and terminal silicate sites or silanols, between adjacent terminal silanols and terminal silicate sites, between water or terminal silanols and hydroxyl groups bonded with interlayer calcium ions. Strong hydrogen bonds are favored to form in C-S-H with high Ca/Si molar ratios. The hydrogen bonding in terminal silicate sites is stronger than those in the paring or bridging silicate sites. New insights into the changes of basal spacing, Ca/Si ratio and H₂O/Si ratio of in the molecular structure of C-S-H are presented based on the mechanism of hydrogen bonding.

Original language	English
Article number	117347
Number of pages	10
Journal	Construction and Building Materials
Volume	233
DOIs	https://doi.org/10.1016/j.conbuildmat.2019.117347
Publication status	Published - 10 Feb 2020

Funding

This research has been financially supported by the National Natural Science Foundation of China (project 51672199 and 51972248), the Fundamental Research Funds for the Central Universities (WUT: 2017-YB-008), National Key Research and Development Program of China (Project 2016YFB0303501), research project BY115J004. We thank Dr. Xiaoyun Li from State Key Laboratory of Silicate Materials for Architectures, Chaofeng He and Yunyun Zou from Shiyanjia lab (www.shiyanjia.com) for assistance with the SSNMR tests. This research has been financially supported by the National Natural Science Foundation of China (project 51672199 and 51972248 ), the Fundamental Research Funds for the Central Universities (WUT: 2017-YB-008 ), National Key Research and Development Program of China ( Project 2016YFB0303501 ), research project BY115J004. We thank Dr. Xiaoyun Li from State Key Laboratory of Silicate Materials for Architectures, Chaofeng He and Yunyun Zou from Shiyanjia lab ( www.shiyanjia.com ) for assistance with the SSNMR tests.

Keywords

Calcium silicate hydrate
First principle calculation
Hydrogen bonding
Solid state NMR

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10.1016/j.conbuildmat.2019.117347

published versionFinal published version, 2.19 MBLicence: TAVERNE

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title = "Understanding hydrogen bonding in calcium silicate hydrate combining solid-state NMR and first principle calculations",

abstract = "Mechanisms of hydrogen bonding and molecular structure in the C-S-H are investigated by combining results of 29Si, 1H solid SSNMR analysis and first principle calculations. First principle calculations for 1H chemical shifts are used to correlate the observed 1H SSNMR spectra with the underlying structure of various hydrogen bonds between different silicon moieties and hydrogen groups in the C-S-H gels. The results show that strong hydrogen bonds are formed between water and terminal silicate sites or silanols, between adjacent terminal silanols and terminal silicate sites, between water or terminal silanols and hydroxyl groups bonded with interlayer calcium ions. Strong hydrogen bonds are favored to form in C-S-H with high Ca/Si molar ratios. The hydrogen bonding in terminal silicate sites is stronger than those in the paring or bridging silicate sites. New insights into the changes of basal spacing, Ca/Si ratio and H2O/Si ratio of in the molecular structure of C-S-H are presented based on the mechanism of hydrogen bonding.",

keywords = "Calcium silicate hydrate, First principle calculation, Hydrogen bonding, Solid state NMR",

author = "Bo Li and Neng Li and H.J.H. Brouwers and Qingliang Yu and Wei Chen",

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AU - Li, Bo

AU - Li, Neng

AU - Brouwers, H.J.H.

AU - Yu, Qingliang

AU - Chen, Wei

PY - 2020/2/10

Y1 - 2020/2/10

N2 - Mechanisms of hydrogen bonding and molecular structure in the C-S-H are investigated by combining results of 29Si, 1H solid SSNMR analysis and first principle calculations. First principle calculations for 1H chemical shifts are used to correlate the observed 1H SSNMR spectra with the underlying structure of various hydrogen bonds between different silicon moieties and hydrogen groups in the C-S-H gels. The results show that strong hydrogen bonds are formed between water and terminal silicate sites or silanols, between adjacent terminal silanols and terminal silicate sites, between water or terminal silanols and hydroxyl groups bonded with interlayer calcium ions. Strong hydrogen bonds are favored to form in C-S-H with high Ca/Si molar ratios. The hydrogen bonding in terminal silicate sites is stronger than those in the paring or bridging silicate sites. New insights into the changes of basal spacing, Ca/Si ratio and H2O/Si ratio of in the molecular structure of C-S-H are presented based on the mechanism of hydrogen bonding.

AB - Mechanisms of hydrogen bonding and molecular structure in the C-S-H are investigated by combining results of 29Si, 1H solid SSNMR analysis and first principle calculations. First principle calculations for 1H chemical shifts are used to correlate the observed 1H SSNMR spectra with the underlying structure of various hydrogen bonds between different silicon moieties and hydrogen groups in the C-S-H gels. The results show that strong hydrogen bonds are formed between water and terminal silicate sites or silanols, between adjacent terminal silanols and terminal silicate sites, between water or terminal silanols and hydroxyl groups bonded with interlayer calcium ions. Strong hydrogen bonds are favored to form in C-S-H with high Ca/Si molar ratios. The hydrogen bonding in terminal silicate sites is stronger than those in the paring or bridging silicate sites. New insights into the changes of basal spacing, Ca/Si ratio and H2O/Si ratio of in the molecular structure of C-S-H are presented based on the mechanism of hydrogen bonding.

KW - Calcium silicate hydrate

KW - First principle calculation

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ER -

Understanding hydrogen bonding in calcium silicate hydrate combining solid-state NMR and first principle calculations

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