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Title: Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation

Abstract

Metallic nickel is known to be an active, but not a selective hydrogenation catalyst for conversion of alkynes to alkenes. On the other hand, nickel oxide is not active. Recently, we have demonstrated that nickel doped into ceria provides an inexpensive catalyst for selective hydrogenation of acetylene in the presence of ethylene. Here, we evaluate various synthesis methods to achieve optimal selective hydrogenation performance. We examined incipient wetness impregnation, coprecipitation, solution combustion, and sol-gel synthesis to study how the method of preparation affects catalytic structure and behavior. Sol-gel synthesis, coprecipitation, and solution combustion synthesis methods favor nickel incorporation into the ceria lattice, while incipient wetness impregnation creates segregated nickel species on the ceria surface. For hydrogenation of acetylene, these nickel surface species lead to poor ethylene selectivity due to ethane and oligomer formation. However, when nickel is incorporated into the ceria lattice, ethane formation is prevented even while achieving 100 % conversion of acetylene. Coke formation is also significantly reduced on these catalysts compared to conventional nanoparticle counterparts. Finally, we conclude that sol-gel synthesis provides the optimal method for creating a uniform dopant distribution within the high surface area ceria.

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [1];  [1];  [4];  [4];  [5];  [5];  [3];  [6];  [1]
  1. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering, and Center for Microengineered Materials
  2. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology; Jingdezhen Ceramic Inst. (China). Dept. of Material Science and Engineering
  3. Fuzhou Univ. (China). State Key Lab. of Photocatalysis on Energy and Environment
  4. Univ. of KwaZulu-Natal, Durban (South Africa). School of Chemistry and Physics, Catalysis Research Group
  5. Univ. of New Mexico, Albuquerque, NM (United States). Center for Stable Isotopes
  6. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry and Chemical Biology
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE
OSTI Identifier:
1530590
Alternate Identifier(s):
OSTI ID: 1494787
Grant/Contract Number:  
FG02-05ER15712
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 11; Journal Issue: 5; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; acetylene hydrogenation; catalyst synthesis; ceria; nickel; selective hydrogenation

Citation Formats

Riley, Christopher, De La Riva, Andrew, Zhou, Shulan, Wan, Qiang, Peterson, Eric, Artyushkova, Kateryna, Farahani, Majid D., Friedrich, Holger B., Burkemper, Laura, Atudorei, Nicu‐Viorel, Lin, Sen, Guo, Hua, and Datye, Abhaya. Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation. United States: N. p., 2019. Web. doi:10.1002/cctc.201801976.
Riley, Christopher, De La Riva, Andrew, Zhou, Shulan, Wan, Qiang, Peterson, Eric, Artyushkova, Kateryna, Farahani, Majid D., Friedrich, Holger B., Burkemper, Laura, Atudorei, Nicu‐Viorel, Lin, Sen, Guo, Hua, & Datye, Abhaya. Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation. United States. doi:10.1002/cctc.201801976.
Riley, Christopher, De La Riva, Andrew, Zhou, Shulan, Wan, Qiang, Peterson, Eric, Artyushkova, Kateryna, Farahani, Majid D., Friedrich, Holger B., Burkemper, Laura, Atudorei, Nicu‐Viorel, Lin, Sen, Guo, Hua, and Datye, Abhaya. Tue . "Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation". United States. doi:10.1002/cctc.201801976. https://www.osti.gov/servlets/purl/1530590.
@article{osti_1530590,
title = {Synthesis of Nickel-Doped Ceria Catalysts for Selective Acetylene Hydrogenation},
author = {Riley, Christopher and De La Riva, Andrew and Zhou, Shulan and Wan, Qiang and Peterson, Eric and Artyushkova, Kateryna and Farahani, Majid D. and Friedrich, Holger B. and Burkemper, Laura and Atudorei, Nicu‐Viorel and Lin, Sen and Guo, Hua and Datye, Abhaya},
abstractNote = {Metallic nickel is known to be an active, but not a selective hydrogenation catalyst for conversion of alkynes to alkenes. On the other hand, nickel oxide is not active. Recently, we have demonstrated that nickel doped into ceria provides an inexpensive catalyst for selective hydrogenation of acetylene in the presence of ethylene. Here, we evaluate various synthesis methods to achieve optimal selective hydrogenation performance. We examined incipient wetness impregnation, coprecipitation, solution combustion, and sol-gel synthesis to study how the method of preparation affects catalytic structure and behavior. Sol-gel synthesis, coprecipitation, and solution combustion synthesis methods favor nickel incorporation into the ceria lattice, while incipient wetness impregnation creates segregated nickel species on the ceria surface. For hydrogenation of acetylene, these nickel surface species lead to poor ethylene selectivity due to ethane and oligomer formation. However, when nickel is incorporated into the ceria lattice, ethane formation is prevented even while achieving 100 % conversion of acetylene. Coke formation is also significantly reduced on these catalysts compared to conventional nanoparticle counterparts. Finally, we conclude that sol-gel synthesis provides the optimal method for creating a uniform dopant distribution within the high surface area ceria.},
doi = {10.1002/cctc.201801976},
journal = {ChemCatChem},
issn = {1867-3880},
number = 5,
volume = 11,
place = {United States},
year = {2019},
month = {1}
}

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