skip to main content

DOE PAGESDOE PAGES

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

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

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., 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.. 2017. "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}
}

Works referenced in this record:

Special points for Brillouin-zone integrations
journal, June 1976
  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

A short review of heterogeneous catalytic process for mixed alcohols synthesis via syngas
journal, September 2009

Mechanism of C2+ oxygenate synthesis on Rh catalysts
journal, March 2005
  • Chuang, Steven S. C.; Stevens, Robert W.; Khatri, Rajesh
  • Topics in Catalysis, Vol. 32, Issue 3-4, p. 225-232
  • DOI: 10.1007/s11244-005-2897-2