Ions Tune Interfacial Water Structure and Modulate Hydrophobic Interactions at Silica Surfaces

Tuladhar, Aashish; Dewan, Shalaka; Pezzotti, Simone; Brigiano, Flavio Siro; Creazzo, Fabrizio; Gaigeot, Marie-Pierre; Borguet, Eric

doi:10.1021/jacs.9b13273

Ions Tune Interfacial Water Structure and Modulate Hydrophobic Interactions at Silica Surfaces

Journal Article · Wed Apr 01 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b13273· OSTI ID:1617295

^[1]; Dewan, Shalaka ^[2]; Pezzotti, Simone ^[3]; Brigiano, Flavio Siro ^[3]; Creazzo, Fabrizio ^[3]; ^[3]; ^[2]

Temple Univ., Philadelphia, PA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Temple Univ., Philadelphia, PA (United States)
Univ. Paris-Saclay, Evry (France)

The structure and ultrafast dynamics of the electric double layer (EDL) are central to chemical reactivity and physical properties at solid/aqueous interfaces. While the Gouy–Chapman–Stern model is widely used to describe EDLs, it is solely based on the macroscopic electrostatic attraction of electrolytes for the charged surfaces. Structure and dynamics in the Stern layer are, however, more complex because of competing effects due to the localized surface charge distribution, surface–solvent–ion correlations, and the interfacial hydrogen bonding environment. Here, we report combined time-resolved vibrational sum frequency generation (TR-vSFG) spectroscopy with ab initio DFT-based molecular dynamics simulations (AIMD/DFT-MD) to get direct access to the molecular-level understanding of how ions change the structure and dynamics of the EDL. We show that innersphere adsorbed ions tune the hydrophobicity of the silica–aqueous interface by shifting the structural makeup in the Stern layer from dominant water–surface interactions to water–water interactions. This drives an initially inhomogeneous interfacial water coordination landscape observed at the neat interface toward a homogeneous, highly interconnected in-plane 2D hydrogen bonding (2D-HB) network at the ionic interface, reminiscent of the canonical, hydrophobic air–water interface. This ion-induced transformation results in a characteristic decrease of the vibrational lifetime (T₁) of excited interfacial O–H stretching modes from T₁ ~ 600 fs to T₁ ~ 250 fs. Hence, we propose that the T₁ determined by TR-vSFG in combination with DFT-MD simulations can be widely used for a quantitative spectroscopic probe of the ion kosmotropic/chaotropic effect at aqueous interfaces as well as of the ion-induced surface hydrophobicity.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1617295

Report Number(s):: PNNL-SA--140244

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 15 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Ions Tune Interfacial Water Structure and Modulate Hydrophobic Interactions at Silica Surfaces

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