The conversion of light hydrocarbons to commodity chemicals under ambient conditions with atmospheric O2 is economically attractive and homogeneous organometallic complexes provide a suitable avenue for this conversion. But, due to the sensitivity of electron-rich organometallic complexes towards O2, an ambient oxidation process with O2 as the oxidant poses a clear challenge. Here, we report the use of an O2-sensitive organometallic catalyst for the selective oxidation of CH4 to CH3OH at ambient conditions with atmospheric O2 as the terminal oxidant. By combining electrochemistry with a nanowire-structured electrode, an O2 concentration gradient was established such that the incompatible reactions of CH4 activation and subsequent oxidation were spatially separated. Equivalent turnovers per catalyst of up to 72,000 were achieved; moreover, compared with a pure homogeneous solution, the kinetic rate of CH4 activation within the nanowire array was enhanced by a factor of 660,000. These results promote future work on the synergistic effects between nanomaterials and homogeneous organometallic catalysts that results in new or enhanced reactivity.

Finding harmony among incompatiblity in the selective oxidation of CH4 to CH3OH with atmospheric O2

2019 Fall National Meeting

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.