Zeolitic-Imidazolate Framework Derived Intermetallic Nickel Zinc Carbide Material as a Selective Catalyst for CO2 to CO Reduction at High Pressure
Abstract
Abstract The conversion of CO 2 into CO is an important step in CO 2 utilization to achieve clean fuels and value‐added chemicals. Herein, we explored the pyrolysis of zeolitic imidazolate framework‐8 (ZIF‐8) loaded with different amounts of Ni 2+ to obtain Ni−Zn carbide (Ni 3 ZnC) embedded in N‐doped carbon. Ni is present in the intermetallic compound, while Zn excess remains on the N‐doped carbon. The Ni 3 ZnC phase catalyzes the selective hydrogenation of CO 2 into CO via the reverse water gas shift reaction, reaching 100 % CO selectivity at ∼30 % CO 2 conversion at 450 °C and atmosphere pressure (CO 2 : H 2 =1 : 4, GHSV=30000 mL g cat −1 h −1 ). The methanation reaction of CO 2 /CO, which is usually favored over Ni catalysts, is suppressed. The selectivity to CO at the expense of CH 4 is related to the stability of chemisorbed CO in the Ni 3 ZnC surface, which is lower compared to Ni surfaces. The Ni 3 ZnC@NC catalyst is selective towards CO over a wide range of conditions, including high pressure, that is usually required for the conversion of CO to hydrocarbons and alcohols via the Fisher‐Tropsch synthesis (FTS) process. Contrarily, a classical Ni/SiOmore »
- Authors:
-
- University of Sao Paulo (Brazil)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Sao Paulo Research Foundation; CNPq; USDOE
- OSTI Identifier:
- 1829501
- Alternate Identifier(s):
- OSTI ID: 1832262
- Report Number(s):
- PNNL-SA-163626
Journal ID: ISSN 1434-1948
- Grant/Contract Number:
- AC05-76RL01830; 2014/50279-4; 142339/2016-4; 306024/2019-5; 465454/2014-3; 444061/2018-5
- Resource Type:
- Accepted Manuscript
- Journal Name:
- European Journal of Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 2021; Journal Issue: 44; Journal ID: ISSN 1434-1948
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Carbon dioxide hydrogenation, Carbides, Intermetallic phases, Zeolitic imidazolate frameworks
Citation Formats
Maluf, Nágila C., Braga, Adriano H., Gothe, Maitê L., Borges, Laís R., Alves, Gustavo S., Gonçalves, Renato V., Szanyi, János, Vidinha, Pedro, and Rossi, Liane M. Zeolitic-Imidazolate Framework Derived Intermetallic Nickel Zinc Carbide Material as a Selective Catalyst for CO2 to CO Reduction at High Pressure. United States: N. p., 2021.
Web. doi:10.1002/ejic.202100530.
Maluf, Nágila C., Braga, Adriano H., Gothe, Maitê L., Borges, Laís R., Alves, Gustavo S., Gonçalves, Renato V., Szanyi, János, Vidinha, Pedro, & Rossi, Liane M. Zeolitic-Imidazolate Framework Derived Intermetallic Nickel Zinc Carbide Material as a Selective Catalyst for CO2 to CO Reduction at High Pressure. United States. https://doi.org/10.1002/ejic.202100530
Maluf, Nágila C., Braga, Adriano H., Gothe, Maitê L., Borges, Laís R., Alves, Gustavo S., Gonçalves, Renato V., Szanyi, János, Vidinha, Pedro, and Rossi, Liane M. Sun .
"Zeolitic-Imidazolate Framework Derived Intermetallic Nickel Zinc Carbide Material as a Selective Catalyst for CO2 to CO Reduction at High Pressure". United States. https://doi.org/10.1002/ejic.202100530. https://www.osti.gov/servlets/purl/1829501.
@article{osti_1829501,
title = {Zeolitic-Imidazolate Framework Derived Intermetallic Nickel Zinc Carbide Material as a Selective Catalyst for CO2 to CO Reduction at High Pressure},
author = {Maluf, Nágila C. and Braga, Adriano H. and Gothe, Maitê L. and Borges, Laís R. and Alves, Gustavo S. and Gonçalves, Renato V. and Szanyi, János and Vidinha, Pedro and Rossi, Liane M.},
abstractNote = {Abstract The conversion of CO 2 into CO is an important step in CO 2 utilization to achieve clean fuels and value‐added chemicals. Herein, we explored the pyrolysis of zeolitic imidazolate framework‐8 (ZIF‐8) loaded with different amounts of Ni 2+ to obtain Ni−Zn carbide (Ni 3 ZnC) embedded in N‐doped carbon. Ni is present in the intermetallic compound, while Zn excess remains on the N‐doped carbon. The Ni 3 ZnC phase catalyzes the selective hydrogenation of CO 2 into CO via the reverse water gas shift reaction, reaching 100 % CO selectivity at ∼30 % CO 2 conversion at 450 °C and atmosphere pressure (CO 2 : H 2 =1 : 4, GHSV=30000 mL g cat −1 h −1 ). The methanation reaction of CO 2 /CO, which is usually favored over Ni catalysts, is suppressed. The selectivity to CO at the expense of CH 4 is related to the stability of chemisorbed CO in the Ni 3 ZnC surface, which is lower compared to Ni surfaces. The Ni 3 ZnC@NC catalyst is selective towards CO over a wide range of conditions, including high pressure, that is usually required for the conversion of CO to hydrocarbons and alcohols via the Fisher‐Tropsch synthesis (FTS) process. Contrarily, a classical Ni/SiO 2 catalyst prepared by impregnation produces CH 4 under high pressure.},
doi = {10.1002/ejic.202100530},
journal = {European Journal of Inorganic Chemistry},
number = 44,
volume = 2021,
place = {United States},
year = {Sun Aug 29 00:00:00 EDT 2021},
month = {Sun Aug 29 00:00:00 EDT 2021}
}
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