Characterization of the Behavior of Hydrogen Species on ZnO Electrode during Electrolytic Reduction of Water

Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China

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Corresponding author: E-mail: zzchem@ustc.edu.cn

摘要

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Abstract: The behavior of hydrogen production on ZnO electrode during the electrolytic reduction of water was investigated by cyclic voltammetry (CV) and cathode polarization experiments combined with in situ Raman and photoluminescence spectroscopy. CV experiments indicate that hydrogen species prefers to diffuse into the ZnO bulk at negative potentials and occupies oxygen vacancies and interstitial sites . Meanwhile, the H₂O reduction is self-enhanced during the electroreduction process, as evidenced by the trace crossing of the CV curves and the chronoamperometric experiment. The influence of the H species on the ZnO electrode during the electrocatalytic processes was characterized by the in situ Raman and photoluminescence spectroscopies. These results help us to understand the hydrogen-related catalytic or electrocatalytic processes on ZnO surfaces.
- Electrocatalysis /
- ZnO /
- Water reduction /
- Interstitial hydrogen

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Figure 1. (a) Cyclic voltammograms (CVs) of ZnO electrode in 0.5 mol/L Na₂SO₄ aqueous electrolyte at different potential ranges. Insets show the photos of ZnO electrode at the indicated potentials. (b) The histogram of ZnO electrode shows the reduction charges per square centimeter (Q_reduction, blue columns) and the oxidation charges per square centimeter (Q_oxidation, red columns) at different scanning potential intervals during the CV processes. Inset shows the current-time plot of ZnO electrode in the range of 0.95 V to −1.05 V during the CV process. (c) The ratio of Q_oxidation/Q_reduction on ZnO electrode is plotted as a function of the scanning potential range.

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Figure 2. CVs of ZnO electrodes in 0.5 mol/L Na₂SO₄ aqueous electrolyte within potential windows of 0.95 V to −0.95 V at various scanning rates.

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Figure 3. The cathodic current vs. time curve of ZnO electrode polarized at −0.85 V for 1000 s.

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Figure 4. SEM images for ZnO electrodes at (a) OCP and –0.85 V polarization of (b) 100 s, (c) 200 s, (d) 400 s, (e) 600 s, (f) 1000 s.

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Figure 5. (a) In situ Raman and (b) PL spectra of ZnO electrodes polarized at –0.85 V for different time. The Raman peaks are assigned by the corresponding vibrational modes (the motion of the dominant atom is indicated by the red arrow).

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