Abstract
Hydrogen donation is the key to supercritical water upgrading of heavy oil, because it benefits light distillate production and inhibits condensation, but the mechanism is still unclear. In this work, an isotope tracing method, combined with Fourier transform infrared spectroscopy and nuclear magnetic resonance spectroscopy analyses, was used to elucidate the hydrogen donation mechanism in supercritical water upgrading of asphaltenes. In asphaltenes upgrading, it was found that the aliphatic carbon at the end of the side chain of asphaltene macromolecules could capture deuterium from supercritical heavy water via free radical reactions, and the deuteration ratio at this position was 11 %. For supercritical water upgrading of vacuum residue which is generally considered as a system of asphaltenes dissolved in maltenes, the existing maltenes enhanced hydrogen donation to asphaltenes. Further, a possible hydrogen donation pathway was proposed. This work provides an in-depth understanding of the hydrogen donation mechanism for supercritical water upgrading.
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