Nitrogen doped carbon catalyst for the oxygen reduction reaction to be used for methane partial oxidation
| Author(s) | Craft, Andrew K | |
| Date Accessioned | 2018-02-19T13:37:37Z | |
| Date Available | 2018-02-19T13:37:37Z | |
| Publication Date | 2017 | |
| SWORD Update | 2017-11-10T14:20:20Z | |
| Abstract | Methane (CH4) is a plentiful, naturally occurring hydrocarbon, and the main constituent of natural gas. Due to its abundance, it has been well studied as both a feedstock for chemical production and as a fuel. Recently, methane has become of interest due to it’s release into the atmosphere as a result of human activities. Rather than capture and use methane, companies opt to flare methane, as it is more environmentally and economically friendly. In 2012, these practices led to over $1 Billion lost in fuel. A recent breakthrough involving the use of hydrogen peroxide (H2O2) in the partial oxidation of methane to liquid chemicals at ambient conditions has been made. This process, used an iron based zeolite catalyst, and moderate concentrations of peroxide. Although peroxide is produced inexpensively industrially, there are cost and safety concerns with shipping the product to the remote fields where it would be used in this process. Nitrogen doped carbon materials have been identified as promising electrocatalysts for the oxygen reduction reaction (ORR). ☐ Here, the synthesis and subsequent testing of a NDC catalyst is reported. KIT-6, a mesoporous silica was used as a hard template, with an ionic liquid being the carbon and nitrogen precursor. Powder x-ray diffraction, N2 adsorption, scanning electron microscopy, and elemental analysis were used to characterize the template and resulting catalyst. Pore size distribution of KIT-6 can be influenced by slight changes in the synthesis procedure. This was utilized in an attempt to change the properties of the final catalyst. Slight changes in the hydrothermal ageing temperature changed the pore distribution in template, and the ECSA was significantly increased as a result. Rotating Disk Electrode (RDE) testing shows that the catalysts have high selectivity (90%) towards H2O2. A RDE is not a production method that can be used industrially. In the best circumstances, it would take over 4 hours to accumulate the required amount of H2O2 used by Hammond et al. Mass transport of the reactants to the surface of the catalyst hinders the overall activity. A flow cell type device can help overcome these limitations by delivering the reactants directly to the catalyst surface. Current densities of 50 mA cm-2 with selectivity around 60% was achieved in the tested flow cell. This device would require ~40 minutes to produce the necessary amount of peroxide to be used if scaled up to 25 cm2. | en_US |
| Advisor | Jiao, Feng | |
| Degree | M.Ch.E. | |
| Department | University of Delaware, Department of Chemical and Biomolecular Engineering | |
| Unique Identifier | 1023575110 | |
| URL | http://udspace.udel.edu/handle/19716/23034 | |
| Language | en | |
| Publisher | University of Delaware | en_US |
| URI | https://search.proquest.com/docview/1972689827?accountid=10457 | |
| Keywords | Pure sciences | en_US |
| Keywords | Applied sciences | en_US |
| Keywords | Carbon | en_US |
| Keywords | Catalyst | en_US |
| Keywords | Methane | en_US |
| Keywords | Nitrogen | en_US |
| Keywords | Oxidation | en_US |
| Keywords | Oxygen | en_US |
| Keywords | Reduction | en_US |
| Title | Nitrogen doped carbon catalyst for the oxygen reduction reaction to be used for methane partial oxidation | en_US |
| Type | Thesis | en_US |