Effects of bubbles on the electrochemical behavior of hydrogen-evolving Si microwire arrays oriented against gravity

Kempler, Paul A.; Coridan, Robert H.; Lewis, Nathan S.

doi:10.1039/d0ee00356e

Effects of bubbles on the electrochemical behavior of hydrogen-evolving Si microwire arrays oriented against gravity

Journal Article · Wed Apr 08 00:00:00 EDT 2020 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d0ee00356e· OSTI ID:1801639

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California Institute of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering; OSTI
Univ. of Arkansas, Fayetteville, AR (United States). Dept. of Chemistry and Biochemistry
California Institute of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering. Beckman Inst.

The size-distribution, coverage, electrochemical impedance, and mass-transport properties of H₂ gas-bubble films were measured for both planar and microwire-array platinized n⁺-Si cathodes performing the hydrogen-evolution reaction in 0.50 M H₂SO₄(aq). Inverted, planar n⁺-Si/Ti/Pt cathodes produced large, stationary bubbles which contributed to substantial increases in ohmic potential drops. In contrast, regardless of orientation, microwire array n⁺-Si/Ti/Pt cathodes exhibited a smaller layer of bubbles on the surface, and the formation of bubbles did not substantially increase the steady-state overpotential for H₂(g) production. Experiments using an electroactive tracer species indicated that even when oriented against gravity, bubbles enhanced mass transport at the electrode surface. Microconvection due to growing and coalescing bubbles dominated effects due to macroconvection of gliding bubbles on Si microwire array cathodes. Electrodes that maintained a large number of small bubbles on the surface simultaneously exhibited low concentrations of dissolved hydrogen and small ohmic potential drops, thus exhibiting the lowest steady-state overpotentials. The results indicate that microstructured electrodes can operate acceptably for unassisted solar-driven water splitting in the absence of external convection and can function regardless of the orientation of the electrode with respect to the gravitational force vector.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0004993

OSTI ID:: 1801639

Alternate ID(s):: OSTI ID: 1630160

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 6 Vol. 13; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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