Effect of current density and sulfuric acid concentration on persulfuric acid generation by boron-doped diamond film anodes

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Abstract

This research investigated the effects of current density and sulfuric acid concentration on the rates of persulfate generation by boron-doped diamond film anodes. Also investigated was the maximum conversion of sulfate to persulfate that could be achieved from electrolysis of sulfuric acid. Experiments were performed in batch systems using a rotating disk electrode (RDE) and a flow-through reactor with parallel plate electrodes. Both the RDE and flow-through experiments showed that there was a linear relationship between persulfate generation rates and current density. Persulfate generation rates became current limited at sulfuric acid concentrations of 2.25 M and above; however, Faradaic efficiencies under current-limited conditions were only ~60 %, and were only weakly dependent on the current density. Persulfate generation rates in the flow-through reactor showed similar dependencies on current density and sulfuric acid concentration as those in the RDE reactor, but were 20-50 % lower. Acid catalyzed and thermal decomposition of persulfate limited the maximum conversion of sulfate to persulfate. A maximum fractional conversion of 78 % was achieved using an initial sulfuric acid concentration of 0.77 M. Surprisingly, this value was independent of the current density over the range of 100-300 mA cm-2.

Original languageEnglish (US)
Pages (from-to)841-848
Number of pages8
JournalJournal of Applied Electrochemistry
Volume44
Issue number7
DOIs
StatePublished - 2014

Fingerprint

Boron
Diamond films
Sulfuric acid
Anodes
Current density
Rotating disks
Acids
Electrodes
Sulfates
Electrolysis
Pyrolysis
Experiments
sulfuric acid

Keywords

  • BDD Anode
  • Boron-doped diamond
  • Electrochemical
  • Electrosynthesis
  • Persulfate
  • Sulfuric acid

ASJC Scopus subject areas

  • Electrochemistry
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

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title = "Effect of current density and sulfuric acid concentration on persulfuric acid generation by boron-doped diamond film anodes",
abstract = "This research investigated the effects of current density and sulfuric acid concentration on the rates of persulfate generation by boron-doped diamond film anodes. Also investigated was the maximum conversion of sulfate to persulfate that could be achieved from electrolysis of sulfuric acid. Experiments were performed in batch systems using a rotating disk electrode (RDE) and a flow-through reactor with parallel plate electrodes. Both the RDE and flow-through experiments showed that there was a linear relationship between persulfate generation rates and current density. Persulfate generation rates became current limited at sulfuric acid concentrations of 2.25 M and above; however, Faradaic efficiencies under current-limited conditions were only ~60 {\%}, and were only weakly dependent on the current density. Persulfate generation rates in the flow-through reactor showed similar dependencies on current density and sulfuric acid concentration as those in the RDE reactor, but were 20-50 {\%} lower. Acid catalyzed and thermal decomposition of persulfate limited the maximum conversion of sulfate to persulfate. A maximum fractional conversion of 78 {\%} was achieved using an initial sulfuric acid concentration of 0.77 M. Surprisingly, this value was independent of the current density over the range of 100-300 mA cm-2.",
keywords = "BDD Anode, Boron-doped diamond, Electrochemical, Electrosynthesis, Persulfate, Sulfuric acid",
author = "Davis, {Jake R.} and Baygents, {James C} and James Farrell",
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AU - Davis, Jake R.

AU - Baygents, James C

AU - Farrell, James

PY - 2014

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N2 - This research investigated the effects of current density and sulfuric acid concentration on the rates of persulfate generation by boron-doped diamond film anodes. Also investigated was the maximum conversion of sulfate to persulfate that could be achieved from electrolysis of sulfuric acid. Experiments were performed in batch systems using a rotating disk electrode (RDE) and a flow-through reactor with parallel plate electrodes. Both the RDE and flow-through experiments showed that there was a linear relationship between persulfate generation rates and current density. Persulfate generation rates became current limited at sulfuric acid concentrations of 2.25 M and above; however, Faradaic efficiencies under current-limited conditions were only ~60 %, and were only weakly dependent on the current density. Persulfate generation rates in the flow-through reactor showed similar dependencies on current density and sulfuric acid concentration as those in the RDE reactor, but were 20-50 % lower. Acid catalyzed and thermal decomposition of persulfate limited the maximum conversion of sulfate to persulfate. A maximum fractional conversion of 78 % was achieved using an initial sulfuric acid concentration of 0.77 M. Surprisingly, this value was independent of the current density over the range of 100-300 mA cm-2.

AB - This research investigated the effects of current density and sulfuric acid concentration on the rates of persulfate generation by boron-doped diamond film anodes. Also investigated was the maximum conversion of sulfate to persulfate that could be achieved from electrolysis of sulfuric acid. Experiments were performed in batch systems using a rotating disk electrode (RDE) and a flow-through reactor with parallel plate electrodes. Both the RDE and flow-through experiments showed that there was a linear relationship between persulfate generation rates and current density. Persulfate generation rates became current limited at sulfuric acid concentrations of 2.25 M and above; however, Faradaic efficiencies under current-limited conditions were only ~60 %, and were only weakly dependent on the current density. Persulfate generation rates in the flow-through reactor showed similar dependencies on current density and sulfuric acid concentration as those in the RDE reactor, but were 20-50 % lower. Acid catalyzed and thermal decomposition of persulfate limited the maximum conversion of sulfate to persulfate. A maximum fractional conversion of 78 % was achieved using an initial sulfuric acid concentration of 0.77 M. Surprisingly, this value was independent of the current density over the range of 100-300 mA cm-2.

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KW - Sulfuric acid

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