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Nanoscale active sites for the hydrogen evolution reaction on low carbon steel
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Yule, Lewis C., Shkirskiy, Viacheslav, Aarons, Jolyon, West, Geoffrey D., Bentley, Cameron Luke, Shollock, Barbara A. and Unwin, Patrick R. (2019) Nanoscale active sites for the hydrogen evolution reaction on low carbon steel. The Journal of Physical Chemistry C . doi:10.1021/acs.jpcc.9b07216 (In Press)
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WRAP-Nanoscale-Active-Sites-Hydrogen-Steel-Yule-2019.pdf - Accepted Version - Requires a PDF viewer. Download (1015Kb) | Preview |
Official URL: http://dx.doi.org/10.1021/acs.jpcc.9b07216
Abstract
To fully elucidate the structural controls on corrosion-related processes at metal surfaces, experimental measurements should correlate and compare directly structure and activity at the scale of surface heterogeneities (e.g., individual grains, grain boundaries, inclusions etc.). For example, the hydrogen evolution reaction (HER), which usually serves as the cathodic counterpart to anodic metal dissolution in acidic media, may be highly sensitive to surface microstructure, highlighting the need for nanoscale-resolution electrochemical techniques. In this study, we employ scanning electrochemical cell microscopy (SECCM) in conjunction with co-located scanning electron microscopy, electron backscatter diffraction, and energy dispersive X-ray spectroscopy to elucidate the relationship between surface structure/composition and HER activity on low carbon steel in aqueous sulfuric acid (pH ≈ 2.3). Through this correlative electrochemical multimicroscopy approach, we show that the HER activity of the low index grains (slightly) decreases in the order (100) > (111) > (101), with grain-dependent free energy of hydrogen adsorption (calculated for the low index planes of iron using density functional theory, DFT) proposed as a tentative explanation for this subtle structural-dependence. More significantly, we show that the HER is greatly facilitated by sub-micron surface defects, specifically grain boundaries and MnS inclusions, directly identifying these heterogeneities as potential “cathodic sites” during (atmospheric) corrosion. This study demonstrates the considerable attributes of correlative SECCM for identifying nanoscale active sites on surfaces, greatly aiding understanding of corrosion and electrocatalytic processes.
| Item Type: | Journal Article | |||||||||||||||||||||
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| Subjects: | Q Science > QC Physics Q Science > QH Natural history T Technology > TA Engineering (General). Civil engineering (General) |
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| Divisions: | Faculty of Science > Chemistry Faculty of Science > Physics Faculty of Science > WMG (Formerly the Warwick Manufacturing Group) |
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| Library of Congress Subject Headings (LCSH): | Metals -- Surfaces , Corrosion and anti-corrosives , Scanning electrochemical microscopy , Hydrogen -- Absorption and adsorption, Density functionals | |||||||||||||||||||||
| Journal or Publication Title: | The Journal of Physical Chemistry C | |||||||||||||||||||||
| Publisher: | American Chemical Society | |||||||||||||||||||||
| ISSN: | 1932-7447 | |||||||||||||||||||||
| Official Date: | 9 September 2019 | |||||||||||||||||||||
| Dates: |
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| Date of first compliant deposit: | 12 September 2019 | |||||||||||||||||||||
| DOI: | 10.1021/acs.jpcc.9b07216 | |||||||||||||||||||||
| Status: | Peer Reviewed | |||||||||||||||||||||
| Publication Status: | In Press | |||||||||||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | |||||||||||||||||||||
| Copyright Holders: | https://doi.org/10.1021/acs.jpcc.9b07216 | |||||||||||||||||||||
| RIOXX Funder/Project Grant: |
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