Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]
Abstract
Here, the low-temperature conversion of methane into value-added products is an appealing goal due to the abundance of methane in the form of natural gas. Industrially, methane is used to produce synthesis gas (syngas), a precursor mixture used heavily in the production of ammonia, methanol, and synthetic fuels. In practice, this mixture is produced via the energy-intensive methane steam reforming reaction at temperatures between 750 and 1450 °C. The exothermic methane partial oxidation reaction stands as an alternative for syngas formation at lower temperatures, especially for gas to liquid fuels applications, yet awaits large-scale implementation due to dangerous operating conditions and temperatures. Using colloidally synthesized Ru catalysts, we identify two unifying rules that govern the low-temperature production of synthesis gas: depletion of oxygen within the catalyst bed and facile RuO2 → Ru reduction kinetics, which is a strong function of supporting material and Ru nanostructure. Using these design rules, we demonstrate the enhanced low-temperature activity of a bifunctional Ru/Pd catalyst which produces synthesis gas at ~400 °C, with nearly complete CH4 conversion and CO selectivity at 670 °C.
- Authors:
-
[2];
[1]
- Stanford Univ., Stanford, CA (United States)
- Stanford Univ., Stanford, 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)
- OSTI Identifier:
- 1471402
- Grant/Contract Number:
- DGE-1656518
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Nano Materials
- Additional Journal Information:
- Journal Volume: 1; Journal Issue: 9; Journal ID: ISSN 2574-0970
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 03 NATURAL GAS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalyst; methane partial oxidation; nanocrystal; ruthenium; syngas
Citation Formats
Goodman, Emmett D., Latimer, Allegra A., Yang, An -Chih, Wu, Liheng, Tahsini, Nadia, Abild-Pedersen, Frank, and Cargnello, Matteo. Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]. United States: N. p., 2018.
Web. doi:10.1021/acsanm.8b01256.
Goodman, Emmett D., Latimer, Allegra A., Yang, An -Chih, Wu, Liheng, Tahsini, Nadia, Abild-Pedersen, Frank, & Cargnello, Matteo. Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]. United States. https://doi.org/10.1021/acsanm.8b01256
Goodman, Emmett D., Latimer, Allegra A., Yang, An -Chih, Wu, Liheng, Tahsini, Nadia, Abild-Pedersen, Frank, and Cargnello, Matteo. Thu .
"Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]". United States. https://doi.org/10.1021/acsanm.8b01256. https://www.osti.gov/servlets/purl/1471402.
@article{osti_1471402,
title = {Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts [Targeting Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts]},
author = {Goodman, Emmett D. and Latimer, Allegra A. and Yang, An -Chih and Wu, Liheng and Tahsini, Nadia and Abild-Pedersen, Frank and Cargnello, Matteo},
abstractNote = {Here, the low-temperature conversion of methane into value-added products is an appealing goal due to the abundance of methane in the form of natural gas. Industrially, methane is used to produce synthesis gas (syngas), a precursor mixture used heavily in the production of ammonia, methanol, and synthetic fuels. In practice, this mixture is produced via the energy-intensive methane steam reforming reaction at temperatures between 750 and 1450 °C. The exothermic methane partial oxidation reaction stands as an alternative for syngas formation at lower temperatures, especially for gas to liquid fuels applications, yet awaits large-scale implementation due to dangerous operating conditions and temperatures. Using colloidally synthesized Ru catalysts, we identify two unifying rules that govern the low-temperature production of synthesis gas: depletion of oxygen within the catalyst bed and facile RuO2 → Ru reduction kinetics, which is a strong function of supporting material and Ru nanostructure. Using these design rules, we demonstrate the enhanced low-temperature activity of a bifunctional Ru/Pd catalyst which produces synthesis gas at ~400 °C, with nearly complete CH4 conversion and CO selectivity at 670 °C.},
doi = {10.1021/acsanm.8b01256},
journal = {ACS Applied Nano Materials},
number = 9,
volume = 1,
place = {United States},
year = {Thu Aug 16 00:00:00 EDT 2018},
month = {Thu Aug 16 00:00:00 EDT 2018}
}
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