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Title: A theoretical explanation of the effect of oxygen poisoning on industrial Haber-Bosch catalysts

Abstract

The Haber-Bosch process has been investigated extensively, however a low-temperature, low-pressure process remains elusive. As has been demonstrated many times, this stems in part from the difficulty of breaking the N-N triple bond. In this work, we highlight an additional reason for the lack of a low-temperature ammonia synthesis process: the effect of oxygen poisoning at low temperature. Using density functional theory (DFT), we have created a new model for the active site of industrial Haber-Bosch catalysts which explicitly includes the potassium promoter. Furthermore, we present a new micro-kinetic model for ammonia synthesis that includes the effect of oxygen poisoning due to trace water content in the input gas stream. Our model agrees well with previous experiments and shows that devising a strategy to avoid oxygen poisoning is crucial to creating a low-temperature Haber-Bosch process. Additionally, the model suggests that using a weaker-binding catalyst is one way to avoid oxygen poisoning if it is impractical to remove all water from the reactor.

Authors:
 [1];  [1];  [2]
  1. Stanford Univ., CA (United States)
  2. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Technical Univ. of Denmark, Lyngby (Denmark)
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); NSF Graduate Research Fellowships Program (GRFP)
OSTI Identifier:
1532512
Grant/Contract Number:  
AC02-76SF00515; DGE-1656518
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 372; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ammonia; Haber-Bosch; Alkali promotion; Kinetic modeling; Catalyst poisoning; Density functional theory

Citation Formats

Rohr, Brian A., Singh, Aayush R., and Nørskov, Jens K. A theoretical explanation of the effect of oxygen poisoning on industrial Haber-Bosch catalysts. United States: N. p., 2019. Web. doi:10.1016/j.jcat.2019.01.042.
Rohr, Brian A., Singh, Aayush R., & Nørskov, Jens K. A theoretical explanation of the effect of oxygen poisoning on industrial Haber-Bosch catalysts. United States. doi:10.1016/j.jcat.2019.01.042.
Rohr, Brian A., Singh, Aayush R., and Nørskov, Jens K. Wed . "A theoretical explanation of the effect of oxygen poisoning on industrial Haber-Bosch catalysts". United States. doi:10.1016/j.jcat.2019.01.042.
@article{osti_1532512,
title = {A theoretical explanation of the effect of oxygen poisoning on industrial Haber-Bosch catalysts},
author = {Rohr, Brian A. and Singh, Aayush R. and Nørskov, Jens K.},
abstractNote = {The Haber-Bosch process has been investigated extensively, however a low-temperature, low-pressure process remains elusive. As has been demonstrated many times, this stems in part from the difficulty of breaking the N-N triple bond. In this work, we highlight an additional reason for the lack of a low-temperature ammonia synthesis process: the effect of oxygen poisoning at low temperature. Using density functional theory (DFT), we have created a new model for the active site of industrial Haber-Bosch catalysts which explicitly includes the potassium promoter. Furthermore, we present a new micro-kinetic model for ammonia synthesis that includes the effect of oxygen poisoning due to trace water content in the input gas stream. Our model agrees well with previous experiments and shows that devising a strategy to avoid oxygen poisoning is crucial to creating a low-temperature Haber-Bosch process. Additionally, the model suggests that using a weaker-binding catalyst is one way to avoid oxygen poisoning if it is impractical to remove all water from the reactor.},
doi = {10.1016/j.jcat.2019.01.042},
journal = {Journal of Catalysis},
number = C,
volume = 372,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
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This content will become publicly available on February 27, 2020
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