Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions

Norton, Angela M.; Kim, Donghun; Zheng, Weiqing; Akter, Nusnin; Xu, Yixin; Tenney, Samuel A.; Vlachos, Dionisios G.; Tsapatsis, Michael; Boscoboinik, J. Anibal

doi:10.1021/acs.jpcc.0c03875

Title: Reversible Formation of Silanol Groups in Two-Dimensional Siliceous Nanomaterials under Mild Hydrothermal Conditions

Journal Article · Sun Jul 26 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c03875· OSTI ID:1670664

Norton, Angela M. ^[1]; Kim, Donghun ^[2]; Zheng, Weiqing ^[3]; Akter, Nusnin ^[4]; Xu, Yixin ^[4];

^[5];

^[1];

^[6];

^[7]

Univ. of Delaware, Newark, DE (United States)
Univ. of Minnesota, Minneapolis, MN (United States); Chonnam National Univ., Gwangju (Korea, Republic of)
Catalysis Center for Energy Innovation, University of Delaware, 221 Academy Street, Newark, Delaware 19716 United States
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of Delaware, Newark, DE (United States); Univ. of Minnesota, Minneapolis, MN (United States); Johns Hopkins Univ., Baltimore, MD (United States)
Univ. of Delaware, Newark, DE (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Monitoring the effects of mild hydrothermal conditions, in situ, on siliceous materials remains challenging using surface science techniques, which often require electrically conductive substrates. The emergence of two-dimensional (2-D) siliceous nanomaterials deposited on metal single crystals overcomes this limitation. Here, we use infrared reflection absorption spectroscopy (IRRAS) to study the effects of mild hydrothermal conditions, in situ, on 2-D model systems, namely, all-Si MFI nanosheets supported on Au(111) and a polymorphous bilayer silicate supported on Ru(0001). We find that the formation of silanol groups (SiOH) occurs at 473 and 573 K under a H₂O pressure of 3 mbar in the MFI nanosheets, but not in the polymorphous bilayer silicate. The effects of mild hydrothermal conditions are reversible in the MFI nanosheets and do not result in framework degradation. Implications shown here provide a fundamental understanding of the impact of mild hydrothermal conditions on the 2-D siliceous nanomaterials and serve as a starting point when considering these effects on three-dimensional (3-D) ones.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; SC0001004

OSTI ID:: 1670664

Report Number(s):: BNL-219914-2020-JAAM

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 33; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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