The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts

Nuoya Yang; Xinyan Liu; Arun S. Asundi; Jens K. Nørskov; Stacey F. Bent

doi:10.1007/s10562-017-2223-1

The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts

Nuoya Yang, Xinyan Liu, Arun S. Asundi, Jens K. Nørskov, Stacey F. Bent^*

^*Corresponding author for this work

Stanford University

Research output: Contribution to journal › Journal article › Research › peer-review

Abstract

Abstract: Alkali metal oxides commonly exist as impurities or promoters in syngas conversion catalysts and can significantly influence the activity and selectivity towards higher oxygenate products. In this study, we investigate the effects of sodium oxide on silica-supported Rh catalysts by experimentally introducing different amounts of sodium and monitoring the change in reactivity and CO adsorption behavior. The experimental results combined with density functional theory (DFT) calculations show that sodium selectively blocks step/defect sites on Rh surfaces, leading to reduced activity but higher C₂ oxygenate selectivity. DFT calculations also suggest that sodium present on Rh terrace sites can facilitate CO dissociation, potentially increasing C₂ oxygenate production. The overall activity and selectivity toward various products can be changed significantly based on the degree of site blocking by the added sodium.

Original language	English
Journal	Catalysis Letters
Volume	148
Issue number	1
Pages (from-to)	289-297
ISSN	1011-372X
DOIs	https://doi.org/10.1007/s10562-017-2223-1
Publication status	Published - 2018
Externally published	Yes

Keywords

Alkali impurity
Alkali promoter
Higher oxygenates synthesis
Rh catalyst
Syngas conversion

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10.1007/s10562-017-2223-1

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title = "The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts",

abstract = "Abstract: Alkali metal oxides commonly exist as impurities or promoters in syngas conversion catalysts and can significantly influence the activity and selectivity towards higher oxygenate products. In this study, we investigate the effects of sodium oxide on silica-supported Rh catalysts by experimentally introducing different amounts of sodium and monitoring the change in reactivity and CO adsorption behavior. The experimental results combined with density functional theory (DFT) calculations show that sodium selectively blocks step/defect sites on Rh surfaces, leading to reduced activity but higher C2 oxygenate selectivity. DFT calculations also suggest that sodium present on Rh terrace sites can facilitate CO dissociation, potentially increasing C2 oxygenate production. The overall activity and selectivity toward various products can be changed significantly based on the degree of site blocking by the added sodium. ",

keywords = "Alkali impurity, Alkali promoter, Higher oxygenates synthesis, Rh catalyst, Syngas conversion",

author = "Nuoya Yang and Xinyan Liu and Asundi, {Arun S.} and N{\o}rskov, {Jens K.} and Bent, {Stacey F.}",

year = "2018",

doi = "10.1007/s10562-017-2223-1",

language = "English",

volume = "148",

pages = "289--297",

journal = "Catalysis Letters",

issn = "1011-372X",

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TY - JOUR

T1 - The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts

AU - Yang, Nuoya

AU - Liu, Xinyan

AU - Asundi, Arun S.

AU - Nørskov, Jens K.

AU - Bent, Stacey F.

PY - 2018

Y1 - 2018

N2 - Abstract: Alkali metal oxides commonly exist as impurities or promoters in syngas conversion catalysts and can significantly influence the activity and selectivity towards higher oxygenate products. In this study, we investigate the effects of sodium oxide on silica-supported Rh catalysts by experimentally introducing different amounts of sodium and monitoring the change in reactivity and CO adsorption behavior. The experimental results combined with density functional theory (DFT) calculations show that sodium selectively blocks step/defect sites on Rh surfaces, leading to reduced activity but higher C2 oxygenate selectivity. DFT calculations also suggest that sodium present on Rh terrace sites can facilitate CO dissociation, potentially increasing C2 oxygenate production. The overall activity and selectivity toward various products can be changed significantly based on the degree of site blocking by the added sodium.

AB - Abstract: Alkali metal oxides commonly exist as impurities or promoters in syngas conversion catalysts and can significantly influence the activity and selectivity towards higher oxygenate products. In this study, we investigate the effects of sodium oxide on silica-supported Rh catalysts by experimentally introducing different amounts of sodium and monitoring the change in reactivity and CO adsorption behavior. The experimental results combined with density functional theory (DFT) calculations show that sodium selectively blocks step/defect sites on Rh surfaces, leading to reduced activity but higher C2 oxygenate selectivity. DFT calculations also suggest that sodium present on Rh terrace sites can facilitate CO dissociation, potentially increasing C2 oxygenate production. The overall activity and selectivity toward various products can be changed significantly based on the degree of site blocking by the added sodium.

KW - Alkali impurity

KW - Alkali promoter

KW - Higher oxygenates synthesis

KW - Rh catalyst

KW - Syngas conversion

U2 - 10.1007/s10562-017-2223-1

DO - 10.1007/s10562-017-2223-1

M3 - Journal article

AN - SCOPUS:85031909334

SN - 1011-372X

VL - 148

SP - 289

EP - 297

JO - Catalysis Letters

JF - Catalysis Letters

IS - 1

ER -

The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts

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