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Title: Water on silicene: A hydrogen bond-autocatalyzed physisorption–chemisorption–dissociation transition

Abstract

A single water molecule is nothing special. However, macroscopic water displays many anomalous properties at interfaces, such as hydrophobicity and hydrophilicity. Although the underlying mechanisms remain elusive, hydrogen bonds between water molecules are expected to play a major role in these interesting phenomena. An important question concerns whether water clusters containing few molecules are qualitatively different from a single molecule. Using the water adsorption behavior as an example and by carefully choosing two-dimensional silicene as the substrate material, we demonstrate that water monomers, dimers, and trimers show distinct adsorption properties at the substrate surface. On silicene, the additional water molecules in dimers and trimers induce a transition from physisorption to chemisorption and then to dissociation, arising from the enhancement of charge transfer and proton transfer processes induced by hydrogen bonding. Such a hydrogen bond autocatalytic effect is expected to have broad applications in metal-free catalysis for the oxygen reduction reaction and water dissociation.

Authors:
 [1];  [2];  [2]
  1. University of Science and Technology of China, Hefei (China). Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics; Lawrence Berkeley National Laboratory, Berkeley, CA (United States). Computational Research Division
  2. University of Science and Technology of China, Hefei (China). Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemical Physics, and Synergetic Innovation Center of Quantum Information and Quantum Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory, Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC).
Sponsoring Org.:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1461963
Resource Type:
Journal Article
Journal Name:
Nano Research
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1998-0124
Country of Publication:
United States
Language:
English

Citation Formats

Hu, Wei, Li, Zhenyu, and Yang, Jinlong. Water on silicene: A hydrogen bond-autocatalyzed physisorption–chemisorption–dissociation transition. United States: N. p., 2017. Web. doi:10.1007/s12274-016-1411-4.
Hu, Wei, Li, Zhenyu, & Yang, Jinlong. Water on silicene: A hydrogen bond-autocatalyzed physisorption–chemisorption–dissociation transition. United States. doi:10.1007/s12274-016-1411-4.
Hu, Wei, Li, Zhenyu, and Yang, Jinlong. Mon . "Water on silicene: A hydrogen bond-autocatalyzed physisorption–chemisorption–dissociation transition". United States. doi:10.1007/s12274-016-1411-4.
@article{osti_1461963,
title = {Water on silicene: A hydrogen bond-autocatalyzed physisorption–chemisorption–dissociation transition},
author = {Hu, Wei and Li, Zhenyu and Yang, Jinlong},
abstractNote = {A single water molecule is nothing special. However, macroscopic water displays many anomalous properties at interfaces, such as hydrophobicity and hydrophilicity. Although the underlying mechanisms remain elusive, hydrogen bonds between water molecules are expected to play a major role in these interesting phenomena. An important question concerns whether water clusters containing few molecules are qualitatively different from a single molecule. Using the water adsorption behavior as an example and by carefully choosing two-dimensional silicene as the substrate material, we demonstrate that water monomers, dimers, and trimers show distinct adsorption properties at the substrate surface. On silicene, the additional water molecules in dimers and trimers induce a transition from physisorption to chemisorption and then to dissociation, arising from the enhancement of charge transfer and proton transfer processes induced by hydrogen bonding. Such a hydrogen bond autocatalytic effect is expected to have broad applications in metal-free catalysis for the oxygen reduction reaction and water dissociation.},
doi = {10.1007/s12274-016-1411-4},
journal = {Nano Research},
issn = {1998-0124},
number = 7,
volume = 10,
place = {United States},
year = {2017},
month = {3}
}

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