期刊
ADVANCED FUNCTIONAL MATERIALS
卷 30, 期 12, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201909262
关键词
incompatible catalysis environments; nanoscale integration; proton transfer; solid-solid interfaces; stacked metal oxide nanolayers; ultrathin silica layer
类别
资金
- Energy & Biosciences Institute through the EBI-Shell program
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
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. Together with the complete O-2 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.
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