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dc.contributor.authorWang, Dabin
dc.contributor.authorAzofra Mesa, Luis
dc.contributor.authorHarb, Moussab
dc.contributor.authorCavallo, Luigi
dc.contributor.authorZhang, Xinyi
dc.contributor.authorSuryanto, Bryan Harry Rahmat
dc.contributor.authorMacFarlane, Douglas Robert
dc.date.accessioned2018-11-21T13:08:11Z
dc.date.available2018-11-21T13:08:11Z
dc.date.issued2018-09-04
dc.identifier.citationWang D, Azofra LM, Harb M, Cavallo L, Zhang X, et al. (2018) Energy-Efficient Nitrogen Reduction to Ammonia at Low Overpotential in Aqueous Electrolyte under Ambient Conditions. ChemSusChem 11: 3416–3422. Available: http://dx.doi.org/10.1002/cssc.201801632.
dc.identifier.issn1864-5631
dc.identifier.doi10.1002/cssc.201801632
dc.identifier.urihttp://hdl.handle.net/10754/629929
dc.description.abstractThe electrochemical nitrogen reduction reaction (NRR) at ambient conditions is a promising alternative to the traditional energy-intensive Haber-Bosch process to produce ammonia. The challenge is to achieve a sufficient energy efficiency, yield rate and selectivity to make the process practical. Herein, we demonstrate that Ruthenium nanoparticles (Ru NPs) enable NRR in 0.01 M HCl aqueous solution at very high energy efficiency, i.e., very low overpotentials. Remarkably, the NRR occurs at potential close to or even above H+/H2 reversible potential, significantly enhancing the NRR selectivity versus the production of H2. NH3 yield rates as high as ~5.5 mg h-1 m-2 at 20°C and 21.4 mg h-1 m-2 at 60°C were achieved at E = -100 mV versus the relative hydrogen electrode (RHE) while a highest Faradaic efficiency of ~5.4% is achievable at E = +10 mV vs. RHE. This work demonstrates the potential use of Ru NPs as an efficient catalyst for NRR at ambient conditions. This ability to catalyse NRR at potentials near or above RHE is imperative in improving the NRR selectivity towards a practical process as well as rendering the H2 viable as by-product. DFT calculations of the mechanism suggest that the efficient NRR process occurring on these predominantly Ru(001) surfaces is catalysed by a dissociative mechanism.
dc.description.sponsorshipThe authors thank Monash Centre for Electron Microscopy (MCEM) for the provision of access to their instruments. L.M.A., M.H. and L.C. acknowledge King Abdullah University of Science and Technology (KAUST) for support. Gratitude is also due to the KAUST Supercomputing Laboratory using the supercomputer Shaheen II for providing the computational resources. This study was supported by an Australian Research Council (ARC) Discovery Grant (DP170102267). D.R.M. is grateful to the ARC for his Australian Laureate Fellowship.
dc.publisherWiley
dc.relation.urlhttps://onlinelibrary.wiley.com/doi/full/10.1002/cssc.201801632
dc.rightsArchived with thanks to ChemSusChem
dc.subjectNitrogen Reduction Ammonia Electrosynthesis
dc.titleEnergy efficient nitrogen reduction to ammonia at low overpotential in aqueous electrolyte under ambient conditions
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalChemSusChem
dc.eprint.versionPost-print
dc.contributor.institutionMonash University; School of Chemsitry; 3800 Clayton AUSTRALIA
dc.contributor.institutionMonash University; School of Chemistry; 13 Rainforest Walk 3800 Clayton AUSTRALIA
dc.contributor.institutionMonash University; Chemistry; 13 Rainforest Walk 3800 Clayton AUSTRALIA
kaust.personAzofra Mesa, Luis
kaust.personHarb, Moussab
kaust.personCavallo, Luigi
refterms.dateFOA2018-11-21T13:33:15Z
kaust.acknowledged.supportUnitSupercomputing Laboratory
kaust.acknowledged.supportUnitSupercomputing Laboratory
dc.date.published-online2018-09-04
dc.date.published-print2018-10-11


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