Photoreduction of CO2 by TiO2 nanocomposites synthesized through reactive direct current magnetron sputter deposition

Le Chen; Michael E. Graham; Gonghu Li; Drew R. Gentner; Nada M. Dimitrijevic; Kimberly A. Gray

doi:10.1016/j.tsf.2009.02.075

Photoreduction of CO₂ by TiO₂ nanocomposites synthesized through reactive direct current magnetron sputter deposition

Le Chen, Michael E. Graham, Gonghu Li, Drew R. Gentner, Nada M. Dimitrijevic, Kimberly A. Gray^*

^*Corresponding author for this work

Civil and Environmental Engineering

Research output: Contribution to journal › Article › peer-review

81 Scopus citations

Abstract

The photoreduction of CO₂ into methane provides a carbon-neutral energy alternative to fossil fuels, but its feasibility requires improvements in the photo-efficiency of materials tailored to this reaction. We hypothesize that mixed phase TiO₂ nano-materials with high interfacial densities are extremely active photocatalysts well suited to solar fuel production by reducing CO₂ to methane and shifting to visible light response. Mixed phase TiO₂ films were synthesized by direct current (DC) magnetron sputtering and characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM) and transmission electron microscope (TEM). Bundles of anatase-rutile nano-columns having high densities of two kinds of interfaces (those among the bundles and those between the columns) are fabricated. Films sputtered at a low deposition angle showed the highest methane yield, compared to TiO₂ fabricated under other sputtering conditions and commercial standard Degussa P25 under UV irradiation. The yield of methane could be significantly increased (~ 12% CO₂ conversion) by increasing the CO₂ to water ratio and temperature (< 100 °C) as a combined effect. These films also displayed a light response strongly shifted into the visible range. This is explained by the creation of non-stoichiometric titania films having unique features that we can potentially tailor to the solar energy applications.

Original language	English (US)
Pages (from-to)	5641-5645
Number of pages	5
Journal	Thin Solid Films
Volume	517
Issue number	19
DOIs	https://doi.org/10.1016/j.tsf.2009.02.075
State	Published - Aug 3 2009

Funding

The financial support provided for this study from the US Department of Energy (DE-FG02-03ER15457/A003 and DE-AC02-06CH11358) is gratefully acknowledged. We also thank researchers Dr. Zoran Saponjic and Dr. Tijana Rajh of Argonne National Laboratory for their kind assistance on EPR spectroscopy. The characterization (XRD, AFM, TEM and SEM) was performed in the MRSEC and NUANCE center at Northwestern University.

Keywords

Carbon dioxide reduction
Sputtering
Titanium dioxide
Transmission electron microscopy

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Surfaces and Interfaces
Surfaces, Coatings and Films
Metals and Alloys
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.tsf.2009.02.075

Cite this

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title = "Photoreduction of CO2 by TiO2 nanocomposites synthesized through reactive direct current magnetron sputter deposition",

abstract = "The photoreduction of CO2 into methane provides a carbon-neutral energy alternative to fossil fuels, but its feasibility requires improvements in the photo-efficiency of materials tailored to this reaction. We hypothesize that mixed phase TiO2 nano-materials with high interfacial densities are extremely active photocatalysts well suited to solar fuel production by reducing CO2 to methane and shifting to visible light response. Mixed phase TiO2 films were synthesized by direct current (DC) magnetron sputtering and characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM) and transmission electron microscope (TEM). Bundles of anatase-rutile nano-columns having high densities of two kinds of interfaces (those among the bundles and those between the columns) are fabricated. Films sputtered at a low deposition angle showed the highest methane yield, compared to TiO2 fabricated under other sputtering conditions and commercial standard Degussa P25 under UV irradiation. The yield of methane could be significantly increased (~ 12% CO2 conversion) by increasing the CO2 to water ratio and temperature (< 100 °C) as a combined effect. These films also displayed a light response strongly shifted into the visible range. This is explained by the creation of non-stoichiometric titania films having unique features that we can potentially tailor to the solar energy applications.",

keywords = "Carbon dioxide reduction, Sputtering, Titanium dioxide, Transmission electron microscopy",

author = "Le Chen and Graham, {Michael E.} and Gonghu Li and Gentner, {Drew R.} and Dimitrijevic, {Nada M.} and Gray, {Kimberly A.}",

note = "Funding Information: The financial support provided for this study from the US Department of Energy (DE-FG02-03ER15457/A003 and DE-AC02-06CH11358) is gratefully acknowledged. We also thank researchers Dr. Zoran Saponjic and Dr. Tijana Rajh of Argonne National Laboratory for their kind assistance on EPR spectroscopy. The characterization (XRD, AFM, TEM and SEM) was performed in the MRSEC and NUANCE center at Northwestern University.",

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AU - Chen, Le

AU - Graham, Michael E.

AU - Li, Gonghu

AU - Gentner, Drew R.

AU - Dimitrijevic, Nada M.

AU - Gray, Kimberly A.

N1 - Funding Information: The financial support provided for this study from the US Department of Energy (DE-FG02-03ER15457/A003 and DE-AC02-06CH11358) is gratefully acknowledged. We also thank researchers Dr. Zoran Saponjic and Dr. Tijana Rajh of Argonne National Laboratory for their kind assistance on EPR spectroscopy. The characterization (XRD, AFM, TEM and SEM) was performed in the MRSEC and NUANCE center at Northwestern University.

PY - 2009/8/3

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N2 - The photoreduction of CO2 into methane provides a carbon-neutral energy alternative to fossil fuels, but its feasibility requires improvements in the photo-efficiency of materials tailored to this reaction. We hypothesize that mixed phase TiO2 nano-materials with high interfacial densities are extremely active photocatalysts well suited to solar fuel production by reducing CO2 to methane and shifting to visible light response. Mixed phase TiO2 films were synthesized by direct current (DC) magnetron sputtering and characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM) and transmission electron microscope (TEM). Bundles of anatase-rutile nano-columns having high densities of two kinds of interfaces (those among the bundles and those between the columns) are fabricated. Films sputtered at a low deposition angle showed the highest methane yield, compared to TiO2 fabricated under other sputtering conditions and commercial standard Degussa P25 under UV irradiation. The yield of methane could be significantly increased (~ 12% CO2 conversion) by increasing the CO2 to water ratio and temperature (< 100 °C) as a combined effect. These films also displayed a light response strongly shifted into the visible range. This is explained by the creation of non-stoichiometric titania films having unique features that we can potentially tailor to the solar energy applications.

AB - The photoreduction of CO2 into methane provides a carbon-neutral energy alternative to fossil fuels, but its feasibility requires improvements in the photo-efficiency of materials tailored to this reaction. We hypothesize that mixed phase TiO2 nano-materials with high interfacial densities are extremely active photocatalysts well suited to solar fuel production by reducing CO2 to methane and shifting to visible light response. Mixed phase TiO2 films were synthesized by direct current (DC) magnetron sputtering and characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM) and transmission electron microscope (TEM). Bundles of anatase-rutile nano-columns having high densities of two kinds of interfaces (those among the bundles and those between the columns) are fabricated. Films sputtered at a low deposition angle showed the highest methane yield, compared to TiO2 fabricated under other sputtering conditions and commercial standard Degussa P25 under UV irradiation. The yield of methane could be significantly increased (~ 12% CO2 conversion) by increasing the CO2 to water ratio and temperature (< 100 °C) as a combined effect. These films also displayed a light response strongly shifted into the visible range. This is explained by the creation of non-stoichiometric titania films having unique features that we can potentially tailor to the solar energy applications.

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