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Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation.

ABSTRACT: Chemical looping methane partial oxidation provides an energy and cost effective route for methane utilization. However, there is considerable CO₂ co-production in current chemical looping systems, rendering a decreased productivity in value-added fuels or chemicals. In this work, we demonstrate that the co-production of CO₂ can be dramatically suppressed in methane partial oxidation reactions using iron oxide nanoparticles embedded in mesoporous silica matrix. We experimentally obtain near 100% CO selectivity in a cyclic redox system at 750-935?°C, which is a significantly lower temperature range than in conventional oxygen carrier systems. Density functional theory calculations elucidate the origins for such selectivity and show that low-coordinated lattice oxygen atoms on the surface of nanoparticles significantly promote Fe-O bond cleavage and CO formation. We envision that embedded nanostructured oxygen carriers have the potential to serve as a general materials platform for redox reactions with nanomaterials at high temperatures.

SUBMITTER: Liu Y

PROVIDER: S-EPMC6890731 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature

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Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation.

Liu Yan Y Qin Lang L Cheng Zhuo Z Goetze Josh W JW Kong Fanhe F Fan Jonathan A JA Fan Liang-Shih LS

Nature communications 20191203 1

Chemical looping methane partial oxidation provides an energy and cost effective route for methane utilization. However, there is considerable CO<sub>2</sub> co-production in current chemical looping systems, rendering a decreased productivity in value-added fuels or chemicals. In this work, we demonstrate that the co-production of CO<sub>2</sub> can be dramatically suppressed in methane partial oxidation reactions using iron oxide nanoparticles embedded in mesoporous silica matrix. We experimen ...[more]

PMID: 31796744

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Project description:Methane and ammonia have to be removed from wastewater treatment effluent in order to discharge it to receiving water bodies. A potential solution for this is a combination of simultaneous ammonia and methane oxidation by anaerobic ammonia oxidation (anammox) bacteria and nitrite/nitrate-dependent anaerobic methane oxidation (N-damo) microorganisms. When applied, these microorganisms will be exposed to oxygen, but little is known about the effect of a low concentration of oxygen on a culture containing these microorganisms. In this study, a stable coculture containing anammox and N-damo microorganisms in a laboratory scale bioreactor was established under oxygen limitation. Membrane inlet mass spectrometry (MIMS) was used to directly measure the in situ simultaneous activity of N-damo, anammox, and aerobic ammonia-oxidizing microorganisms. In addition, batch tests revealed that the bioreactor also harbored aerobic methanotrophs and anaerobic methanogens. Together with fluorescence in situ hybridization (FISH) analysis and metagenomics, these results indicate that the combination of N-damo and anammox activity under the continuous supply of limiting oxygen concentrations is feasible and can be implemented for the removal of methane and ammonia from anaerobic digester effluents. IMPORTANCE Nitrogen in wastewater leads to eutrophication of the receiving water bodies, and methane is a potent greenhouse gas; it is therefore important that these are removed from wastewater. A potential solution for the simultaneous removal of nitrogenous compounds and methane is the application of a combination of nitrite/nitrate-dependent methane oxidation (N-damo) and anaerobic ammonia oxidation (annamox). In order to do so, it is important to investigate the effect of oxygen on these two anaerobic processes. In this study, we investigate the effect of a continuous oxygen supply on the activity of an anaerobic methane- and ammonia-oxidizing coculture. The findings presented in this study are important for the potential application of these two microbial processes in wastewater treatment.

Dataset Information

Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation.

Publications

Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation.

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