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Title: Operando Atomic Force Microscopy Reveals Mechanics of Structural Water Driven Battery-to-Pseudocapacitor Transition

The presence of structural water in tungsten oxides leads to a transition in the energy storage mechanism from battery-type intercalation (limited by solid state diffusion) to pseudocapacitance (limited by surface kinetics). Here, we demonstrate that these electrochemical mechanisms are linked to the mechanical response of the materials during intercalation of protons and present a pathway to utilize the mechanical coupling for local studies of electrochemistry. Operando atomic force microscopy dilatometry is used to measure the deformation of redox-active energy storage materials and to link the local nanoscale deformation to the electrochemical redox process. Here, this technique reveals that the local mechanical deformation of the hydrated tungsten oxide is smaller and more gradual than the anhydrous oxide and occurs without hysteresis during the intercalation and deintercalation processes. The ability of layered materials with confined structural water to minimize mechanical deformation likely contributes to their fast energy storage kinetics.
Authors:
 [1] ;  [1] ;  [2] ;  [2] ;  [1] ;  [3] ; ORCiD logo [2] ; ORCiD logo [1]
  1. North Carolina State Univ., Raleigh, NC (United States). Dept. of Materials Science & Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  3. Texas A & M Univ., College Station, TX (United States). Dept. of Mechanical Engineering
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 6; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; atomic force microscopy; energy storage; interlayer engineering; nanoconfined water; transition metal oxides
OSTI Identifier:
1495969

Wang, Ruocun, Mitchell, James B., Gao, Qiang, Tsai, Wan-Yu, Boyd, Shelby, Pharr, Matt, Balke, Nina, and Augustyn, Veronica. Operando Atomic Force Microscopy Reveals Mechanics of Structural Water Driven Battery-to-Pseudocapacitor Transition. United States: N. p., Web. doi:10.1021/acsnano.8b02273.
Wang, Ruocun, Mitchell, James B., Gao, Qiang, Tsai, Wan-Yu, Boyd, Shelby, Pharr, Matt, Balke, Nina, & Augustyn, Veronica. Operando Atomic Force Microscopy Reveals Mechanics of Structural Water Driven Battery-to-Pseudocapacitor Transition. United States. doi:10.1021/acsnano.8b02273.
Wang, Ruocun, Mitchell, James B., Gao, Qiang, Tsai, Wan-Yu, Boyd, Shelby, Pharr, Matt, Balke, Nina, and Augustyn, Veronica. 2018. "Operando Atomic Force Microscopy Reveals Mechanics of Structural Water Driven Battery-to-Pseudocapacitor Transition". United States. doi:10.1021/acsnano.8b02273.
@article{osti_1495969,
title = {Operando Atomic Force Microscopy Reveals Mechanics of Structural Water Driven Battery-to-Pseudocapacitor Transition},
author = {Wang, Ruocun and Mitchell, James B. and Gao, Qiang and Tsai, Wan-Yu and Boyd, Shelby and Pharr, Matt and Balke, Nina and Augustyn, Veronica},
abstractNote = {The presence of structural water in tungsten oxides leads to a transition in the energy storage mechanism from battery-type intercalation (limited by solid state diffusion) to pseudocapacitance (limited by surface kinetics). Here, we demonstrate that these electrochemical mechanisms are linked to the mechanical response of the materials during intercalation of protons and present a pathway to utilize the mechanical coupling for local studies of electrochemistry. Operando atomic force microscopy dilatometry is used to measure the deformation of redox-active energy storage materials and to link the local nanoscale deformation to the electrochemical redox process. Here, this technique reveals that the local mechanical deformation of the hydrated tungsten oxide is smaller and more gradual than the anhydrous oxide and occurs without hysteresis during the intercalation and deintercalation processes. The ability of layered materials with confined structural water to minimize mechanical deformation likely contributes to their fast energy storage kinetics.},
doi = {10.1021/acsnano.8b02273},
journal = {ACS Nano},
number = 6,
volume = 12,
place = {United States},
year = {2018},
month = {5}
}