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

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 C 2 oxygenate selectivity. DFT calculations also suggest that sodium present on Rh terrace sites can facilitate CO dissociation, potentially increasing C 2 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.

Authors:
 [1];  [2];  [1];  [2];  [1]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1427466
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Letters
Additional Journal Information:
Journal Volume: 148; Journal Issue: 1; Journal ID: ISSN 1011-372X
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Nuoya, Liu, Xinyan, Asundi, Arun S., Nørskov, Jens K., and Bent, Stacey F. The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts. United States: N. p., 2017. Web. doi:10.1007/s10562-017-2223-1.
Yang, Nuoya, Liu, Xinyan, Asundi, Arun S., Nørskov, Jens K., & Bent, Stacey F. The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts. United States. doi:10.1007/s10562-017-2223-1.
Yang, Nuoya, Liu, Xinyan, Asundi, Arun S., Nørskov, Jens K., and Bent, Stacey F. Mon . "The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts". United States. doi:10.1007/s10562-017-2223-1. https://www.osti.gov/servlets/purl/1427466.
@article{osti_1427466,
title = {The Role of Sodium in Tuning Product Distribution in Syngas Conversion by Rh Catalysts},
author = {Yang, Nuoya and Liu, Xinyan and Asundi, Arun S. and Nørskov, Jens K. and Bent, Stacey F.},
abstractNote = {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.},
doi = {10.1007/s10562-017-2223-1},
journal = {Catalysis Letters},
number = 1,
volume = 148,
place = {United States},
year = {2017},
month = {10}
}

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