Cathodic NH4+leaching of nitrogen impurities in CoMo thin-film electrodes in aqueous acidic solutions

Weilai Yu, Pakpoom Buabthong, Carlos G. Read, Nathan F. Dalleska, Nathan S. Lewis, Hans Joachim Lewerenz, Harry B. Gray, Katharina Brinkert

Research output: Contribution to journalArticlepeer-review

Abstract

Electrocatalytic reduction of dinitrogen (N2) to ammonium (NH4+) in acidic aqueous solutions was investigated at ambient temperature and pressure using a cobalt-molybdenum (CoMo) thin-film electrode prepared by magnetron reactive sputtering. Increased concentrations of ammonium ions (NH4+) were consistently detected in the electrolyte using ion chromatography (IC) after constant-potential electrolysis at various potentials (≤−0.29 Vvs.RHE). Using a newly developed analytical method based on ammonia derivatization, performing the experiments with15N2-labelled gas led however to the detection of increased14NH4+concentrations instead of15NH4+. X-ray photoelectron spectroscopic (XPS) analysis of the electrode surface revealed the presence of Mo-N and Mo-NHxspecies. Several contamination sources were identified that led to substantial increases in the concentration of ammonium ions, including15NH3impurities in15N2gas. The observed ammonium concentrations can be consistently ascribed to leaching of nitrogen (14N) impurities incorporated in the CoMo film during the sputtering process. Researchers in the field are therefore urged to adopt extended protocols to identify and eliminate sources of ammonia contamination and to very carefully monitor the ammonium concentrations in each experimental step.

Original languageEnglish
Pages (from-to)5080-5087
Number of pages8
JournalSustainable Energy and Fuels
Volume4
Issue number10
DOIs
Publication statusPublished - Oct 2020

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology

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