Ultrathin Amorphous Silica Membrane Enhances Proton Transfer across Solid-to-Solid Interfaces of Stacked Metal Oxide Nanolayers while Blocking Oxygen
Abstract
A large jump of proton transfer rates across solid-to-solid interfaces by inserting an ultrathin amorphous silica layer into stacked metal oxide nanolayers is discovered using electrochemical impedance spectroscopy and Fourier-transform infrared reflection absorption spectroscopy (FT-IRRAS). The triple stacked nanolayers of Co3O4, SiO2, and TiO2 prepared by atomic layer deposition (ALD) enable a proton flux of 2400 ± 60 s-1 nm-2 (pH 4, room temperature), while a single TiO2 (5 nm) layer exhibits a threefold lower flux of 830 s-1 nm-2. Based on FT-IRRAS measurements, this remarkable enhancement is proposed to originate from the sandwiched silica layer forming interfacial SiOTi and SiOCo linkages to TiO2 and Co3O4 nanolayers, respectively, with the O bridges providing fast H+ hopping pathways across the solid-to-solid interfaces. Finally, together with the complete O2 impermeability of a 2 nm ALD-grown SiO2 layer, the high flux for proton transport across multi-stack metal oxide layers opens up the integration of incompatible catalytic environments to form functional nanoscale assemblies such as artificial photosystems for CO2 reduction by H2O.
- Authors:
-
[1]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1598525
- Alternate Identifier(s):
- OSTI ID: 1598060
- Grant/Contract Number:
- AC02-05CH11231; AC02‐05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 12; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; incompatible catalysis environments; nanoscale integration; proton transfer; solid-solid interfaces; stacked metal oxide nanolayers; ultrathin silica layer
Citation Formats
Jo, Won Jun, Katsoukis, Georgios, and Frei, Heinz. Ultrathin Amorphous Silica Membrane Enhances Proton Transfer across Solid-to-Solid Interfaces of Stacked Metal Oxide Nanolayers while Blocking Oxygen. United States: N. p., 2020.
Web. doi:10.1002/adfm.201909262.
Jo, Won Jun, Katsoukis, Georgios, & Frei, Heinz. Ultrathin Amorphous Silica Membrane Enhances Proton Transfer across Solid-to-Solid Interfaces of Stacked Metal Oxide Nanolayers while Blocking Oxygen. United States. https://doi.org/10.1002/adfm.201909262
Jo, Won Jun, Katsoukis, Georgios, and Frei, Heinz. Thu .
"Ultrathin Amorphous Silica Membrane Enhances Proton Transfer across Solid-to-Solid Interfaces of Stacked Metal Oxide Nanolayers while Blocking Oxygen". United States. https://doi.org/10.1002/adfm.201909262. https://www.osti.gov/servlets/purl/1598525.
@article{osti_1598525,
title = {Ultrathin Amorphous Silica Membrane Enhances Proton Transfer across Solid-to-Solid Interfaces of Stacked Metal Oxide Nanolayers while Blocking Oxygen},
author = {Jo, Won Jun and Katsoukis, Georgios and Frei, Heinz},
abstractNote = {A large jump of proton transfer rates across solid-to-solid interfaces by inserting an ultrathin amorphous silica layer into stacked metal oxide nanolayers is discovered using electrochemical impedance spectroscopy and Fourier-transform infrared reflection absorption spectroscopy (FT-IRRAS). The triple stacked nanolayers of Co3O4, SiO2, and TiO2 prepared by atomic layer deposition (ALD) enable a proton flux of 2400 ± 60 s-1 nm-2 (pH 4, room temperature), while a single TiO2 (5 nm) layer exhibits a threefold lower flux of 830 s-1 nm-2. Based on FT-IRRAS measurements, this remarkable enhancement is proposed to originate from the sandwiched silica layer forming interfacial SiOTi and SiOCo linkages to TiO2 and Co3O4 nanolayers, respectively, with the O bridges providing fast H+ hopping pathways across the solid-to-solid interfaces. Finally, together with the complete O2 impermeability of a 2 nm ALD-grown SiO2 layer, the high flux for proton transport across multi-stack metal oxide layers opens up the integration of incompatible catalytic environments to form functional nanoscale assemblies such as artificial photosystems for CO2 reduction by H2O.},
doi = {10.1002/adfm.201909262},
journal = {Advanced Functional Materials},
number = 12,
volume = 30,
place = {United States},
year = {Thu Feb 06 00:00:00 EST 2020},
month = {Thu Feb 06 00:00:00 EST 2020}
}
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