Journal article
Removal of Carbon Contaminants Enables Reliable Surface Enhanced Raman Detection of CO2 Reduction Intermediates on Gold Electrodes
Electrochimica acta, Vol.578(December 2026), 149795
09/02/2026
DOI: 10.1016/j.electacta.2026.149795
Abstract
•Treating electrochemically roughened gold with piranha solution removes carbon.•Piranha treatment is able to preserving SERS.•Piranha treatment reduces peak shift variation by 70%.•Without appropriate cleaning, adventitious carbon leads to spurious Raman bands.•We identify key carbon dioxide reduction intermediates on gold.
Adventitious carbon contamination severely compromises the reliability and reproducibility of surface-enhanced Raman spectroscopy (SERS), leading to spectral interference and potential misinterpretation of reaction mechanisms. Here, we demonstrate that piranha solution (3:1, H2SO4:H2O2) removes adventitious carbon from electrochemically roughened gold (Au) electrodes while preserving SERS activity, achieving up to 70% reduction in peak shift variation compared to untreated surfaces. Using perchlorate and thionine as probe molecules, we show that piranha cleaning enables detection of all vibrational modes with unprecedented reproducibility (standard deviation < 2.7 cm−1). This enhanced spectral fidelity allows us to identify, for the first time using SERS, key carbon dioxide reduction reaction (CO2RR) intermediates on Au: *COOH (1030 cm−1) and *COO− (1150 cm−1). Importantly, we show that without appropriate cleaning, adventitious carbon produces Raman peaks easily misinterpreted as CO2RR intermediates, including spurious CO bands at 2125 cm−1 and carboxylate-like features at 1300 to 1600 cm−1. Our cleaning protocol establishes a foundation for reliable SERS-based mechanistic studies in electrocatalysis with immediate applications to energy conversion research.
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Details
- Title: Subtitle
- Removal of Carbon Contaminants Enables Reliable Surface Enhanced Raman Detection of CO2 Reduction Intermediates on Gold Electrodes
- Creators
- Wendy Yu - University of MichiganHarsh Agarwal - University of MichiganJacob Fields - University of IowaJames Akinola - University of MichiganMartin Moskovits - University of California, Santa BarbaraSyed Mubeen - University of IowaNirala Singh - University of Michigan
- Resource Type
- Journal article
- Publication Details
- Electrochimica acta, Vol.578(December 2026), 149795
- DOI
- 10.1016/j.electacta.2026.149795
- ISSN
- 0013-4686
- eISSN
- 1873-3859
- Publisher
- Elsevier Ltd
- Grant note
- Department of Energy's: DE-FE0031704 Army Research Office and Army Research Laboratory (ARL): W911NF-21-1-0149 National Science Foundation (NSF) Graduate Research Fellowship Program (GRFP) NSF: 2320929
We would like to acknowledge Prof. Adam Matzger, Dr. Venky Prabhakaran, Dr. Talshyn Begildayeva, and Dr. Chih-Feng Wang for insightful discussions. H.A., J.F., M.M., S.M, and N.S. acknowledge funding by Department of Energy's grant number DE-FE0031704. J.A. and W.Y. acknowledge support from the Army Research Office and Army Research Laboratory (ARL) under Grant No W911NF-21-1-0149. W.Y. acknowledge funding support from the National Science Foundation (NSF) Graduate Research Fellowship Program (GRFP). The views and conclusions contained in this document are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the Army Research Office, ARL, or the U.S. Government. The U.S. Government is authorized to reproduce and distribute reprints for Government purposes notwithstanding any copyright notation herein. N.S. acknowledges NSF Grant No 2320929.
- Language
- English
- Date published
- 09/02/2026
- Academic Unit
- Civil and Environmental Engineering; Chemical and Biochemical Engineering
- Record Identifier
- 9985220941402771
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