Plasmon-enhanced reverse water gas shift reaction over oxide supported Au catalysts

Aniruddha A. Upadhye; Insoo Ro; Xu Zeng; Hyung Ju Kim; Isabel Tejedor; Marc A. Anderson; James A. Dumesic; George W. Huber

doi:10.1039/c4cy01183j

Plasmon-enhanced reverse water gas shift reaction over oxide supported Au catalysts

Aniruddha A. Upadhye, Insoo Ro, Xu Zeng, Hyung Ju Kim, Isabel Tejedor, Marc A. Anderson, James A. Dumesic, George W. Huber

Dept. of Chemical and Biomolecular Engineering

University of Wisconsin - Madison

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

111 Scopus citations

Abstract

We show that localized surface plasmon resonance (LSPR) can enhance the catalytic activities of different oxide-supported Au catalysts for the reverse water gas shift (RWGS) reaction. Oxide-supported Au catalysts showed 30 to 1300% higher activity for RWGS under visible light compared to dark conditions. Au/TiO₂ catalyst prepared by the deposition-precipitation (DP) method with 3.5 nm average Au particle size showed the highest activity for the RWGS reaction. Visible light is converted into chemical energy for this reaction with up to a 5% overall efficiency. A shift in the apparent activation energy (from 47 kJ mol^-1 in dark to 35 kJ mol^-1 in light) and apparent reaction order with respect to CO₂ (from 0.5 in dark to 1.0 in light) occurs due to the LSPR. Our kinetic results indicate that the LSPR increases the rate of either the hydroxyl hydrogenation or carboxyl decomposition more than any other steps in the reaction network.

Original language	English
Pages (from-to)	2590-2601
Number of pages	12
Journal	Catalysis Science and Technology
Volume	5
Issue number	5
DOIs	https://doi.org/10.1039/c4cy01183j
State	Published - 1 May 2015

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title = "Plasmon-enhanced reverse water gas shift reaction over oxide supported Au catalysts",

abstract = "We show that localized surface plasmon resonance (LSPR) can enhance the catalytic activities of different oxide-supported Au catalysts for the reverse water gas shift (RWGS) reaction. Oxide-supported Au catalysts showed 30 to 1300\% higher activity for RWGS under visible light compared to dark conditions. Au/TiO2 catalyst prepared by the deposition-precipitation (DP) method with 3.5 nm average Au particle size showed the highest activity for the RWGS reaction. Visible light is converted into chemical energy for this reaction with up to a 5\% overall efficiency. A shift in the apparent activation energy (from 47 kJ mol-1 in dark to 35 kJ mol-1 in light) and apparent reaction order with respect to CO2 (from 0.5 in dark to 1.0 in light) occurs due to the LSPR. Our kinetic results indicate that the LSPR increases the rate of either the hydroxyl hydrogenation or carboxyl decomposition more than any other steps in the reaction network.",

author = "Upadhye, \{Aniruddha A.\} and Insoo Ro and Xu Zeng and Kim, \{Hyung Ju\} and Isabel Tejedor and Anderson, \{Marc A.\} and Dumesic, \{James A.\} and Huber, \{George W.\}",

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year = "2015",

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doi = "10.1039/c4cy01183j",

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T1 - Plasmon-enhanced reverse water gas shift reaction over oxide supported Au catalysts

AU - Upadhye, Aniruddha A.

AU - Ro, Insoo

AU - Zeng, Xu

AU - Kim, Hyung Ju

AU - Tejedor, Isabel

AU - Anderson, Marc A.

AU - Dumesic, James A.

AU - Huber, George W.

PY - 2015/5/1

Y1 - 2015/5/1

N2 - We show that localized surface plasmon resonance (LSPR) can enhance the catalytic activities of different oxide-supported Au catalysts for the reverse water gas shift (RWGS) reaction. Oxide-supported Au catalysts showed 30 to 1300% higher activity for RWGS under visible light compared to dark conditions. Au/TiO2 catalyst prepared by the deposition-precipitation (DP) method with 3.5 nm average Au particle size showed the highest activity for the RWGS reaction. Visible light is converted into chemical energy for this reaction with up to a 5% overall efficiency. A shift in the apparent activation energy (from 47 kJ mol-1 in dark to 35 kJ mol-1 in light) and apparent reaction order with respect to CO2 (from 0.5 in dark to 1.0 in light) occurs due to the LSPR. Our kinetic results indicate that the LSPR increases the rate of either the hydroxyl hydrogenation or carboxyl decomposition more than any other steps in the reaction network.

AB - We show that localized surface plasmon resonance (LSPR) can enhance the catalytic activities of different oxide-supported Au catalysts for the reverse water gas shift (RWGS) reaction. Oxide-supported Au catalysts showed 30 to 1300% higher activity for RWGS under visible light compared to dark conditions. Au/TiO2 catalyst prepared by the deposition-precipitation (DP) method with 3.5 nm average Au particle size showed the highest activity for the RWGS reaction. Visible light is converted into chemical energy for this reaction with up to a 5% overall efficiency. A shift in the apparent activation energy (from 47 kJ mol-1 in dark to 35 kJ mol-1 in light) and apparent reaction order with respect to CO2 (from 0.5 in dark to 1.0 in light) occurs due to the LSPR. Our kinetic results indicate that the LSPR increases the rate of either the hydroxyl hydrogenation or carboxyl decomposition more than any other steps in the reaction network.

UR - http://www.scopus.com/inward/record.url?scp=84928910576&partnerID=8YFLogxK

U2 - 10.1039/c4cy01183j

DO - 10.1039/c4cy01183j

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VL - 5

SP - 2590

EP - 2601

JO - Catalysis Science and Technology

JF - Catalysis Science and Technology

IS - 5

ER -

Plasmon-enhanced reverse water gas shift reaction over oxide supported Au catalysts

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