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Title: 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 Co 3O 4, SiO 2, and TiO 2 prepared by atomic layer deposition (ALD) enable a proton flux of 2400 ± 60 s -1 nm -2 (pH 4, room temperature), while a single TiO 2 (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 TiO 2 and Co 3O 4 nanolayers, respectively, with the O bridges providing fast H + hopping pathways across the solid-to-solid interfaces. Finally, together with the complete O 2 impermeability of a 2 nm ALD-grown SiO 2 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 CO 2 reduction by H 2O.

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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 Name: Advanced Functional Materials]; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
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. doi: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. doi:10.1002/adfm.201909262.
@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 = ,
volume = ,
place = {United States},
year = {2020},
month = {2}
}

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