Journal
CHEMICAL ENGINEERING JOURNAL
Volume 383, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.123157
Keywords
Electrodeless plating; Crystal facet; Nitrate; Selectivity; Electrode potential
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Funding
- Ministry of Science and Technology, Taiwan
- MOST [107-2221-E-110-001-MY3]
- US NSF IOA [1632899]
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Cu/Ni composite electrodes were prepared and studied for the electrochemical reduction of nitrate in aqueous solutions. Electrodeless plating technique, with tartrate as chelatant and formaldehyde as reducing agent, enabled the in-situ incorporation of Cu nanoparticles into the open-pore structured Ni foam to form Cu-Ni composite electrodes. X-ray diffractometer (XRD) and scanning electron microscopy (SEM) revealed that the crystal facet and grain morphology of Cu nanoparticles was closely controlled by the plating time and played a significant role in nitrate reduction and nitrogen selectivity. Cyclic voltammetry provided information on the electron transfer between surface nitrogen species and Cu/Ni electrodes. Electrochemical nitrate reduction was initiated at the onset potential of Cu(0)/Cu(I) redox reaction over a potential window of -0.6 V to -1.2 V. The preferential Cu{1 1 1} facet orientation improved the electron transfer process. Batch kinetics studies at constant current and potential showed that specific adsorption of nitrate and nitrite on the Cu{1 1 1} facet was critical to efficient electrochemical nitrate reduction. Moreover, the conversion of nitrogenous byproduct was potential-dependent. Results showed that N-2 selectivity was high (55.6%) at low overpotential (i.e.,>=-0.6 V vs. Hg/HgO. At high overpotential (i.e,<-0.6 V) there was complete of NO3- reduction with NH4+ as major byproduct.
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