Abstract
Syngas produced through gasification of carbonaceous materials provided a gateway to a host of processes for the production of various chemicals including transportation fuels. The basis of the production of gasoline and diesel-like fuels is the Fischer Tropsch Synthesis (FTS) process. It has been argued that only transition metal catalysts (usually Co or Fe) are active toward the CO hydrogenation and subsequent chain growth in the presence of hydrogen. In this paper, we demonstrate that carbon nanotube (CNT) surfaces are also capable of hydro-deoxygenating carbon monoxide and producing long chain hydrocarbons similar to that obtained through the FTS but with orders of magnitude higher activity than the present state-of-the-art FTS catalysts. Using advanced experimental tools such as XPS and microscopy techniques to characterize CNTs, CeO functional groups have been identified as the active sites for the enhanced catalytic activity. Furthermore, quantum Density Functional Theory (DFT) calculations confirm that CeO groups (on CNT surfaces) could indeed be catalytically active towards reduction of CO with H2, and capable of sustaining chain growth. These findings now open a new paradigm for CNT-based hydrogenation catalysts and constitute a defining point for obtaining clean, earth abundant, alternative fuels through the use of efficient and renewable catalyst.
Original language | English |
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Pages (from-to) | 274-284 |
Number of pages | 11 |
Journal | Carbon |
Volume | 121 |
DOIs | |
State | Published - Sep 2017 |
Funding
This research was made possible with support, in part, by the Illinois Department of Commerce and Economic Opportunity (08-1/ER6, 10/7B-5, 12/7D-2) through the Office of Coal Development and the Illinois Clean Coal Institute and a grant from the National Science Foundation (1133117). The authors also acknowledge the financial support provided by the Office of Research and Development (ORDA) at SIUC through faculty start-up funds and a seed grant. MT thanks JST-Japan for funding the Research Center for Exotic NanoCarbons, under the Japanese regional Innovation Strategy Program by the Excellence.
Funders | Funder number |
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JST-Japan | |
ORDA | |
Office of Coal Development | |
SIUC | |
National Science Foundation | |
Directorate for Engineering | 1133117 |
Illinois Department of Commerce and Economic Opportunity | 12/7D-2, 10/7B-5, 08-1/ER6 |
Clean Coal | |
Office of Research and Development |
Keywords
- CNT
- Catalysis
- DFT
- Hydro-deoxygenation
- XTL