Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide
Abstract Water electro-oxidation to form H2O2 is an important way to produce H2O2 which is widely applied in industry. However, its mechanism is under debate and HO(ads), hydroxyl group adsorbed onto the surface of the electrode, is regarded as an important intermediate. Herein, we study the mechani...
Saved in:
| Main Authors: | , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2024-10-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-53134-3 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1850181539212558336 |
|---|---|
| author | Heng Zhu Ximei Lv Yuexu Wu Wentao Wang Yuping Wu Shicheng Yan Yuhui Chen |
| author_facet | Heng Zhu Ximei Lv Yuexu Wu Wentao Wang Yuping Wu Shicheng Yan Yuhui Chen |
| author_sort | Heng Zhu |
| collection | DOAJ |
| description | Abstract Water electro-oxidation to form H2O2 is an important way to produce H2O2 which is widely applied in industry. However, its mechanism is under debate and HO(ads), hydroxyl group adsorbed onto the surface of the electrode, is regarded as an important intermediate. Herein, we study the mechanism of water oxidation to H2O2 at Pt electrode using in-situ Raman spectroscopy and differential electrochemical mass spectroscopy and find peroxide bond mainly originated from the coupling of two CO3 2- via a C2O6 2- intermediate. By quantifying the 18O isotope in the product, we find that 93% of H2O2 was formed via the CO3 2- coupling route and 7% of H2O2 is from OH(ads)-CO3 •− route. The OH(ads)-OH(ads) coupling route has a negligible contribution. The comparison of various electrodes shows that the strong adsorption of CO3(ads) at the electrode surface is essential. Combining with a commercial cathode catalyst to produce H2O2 during oxygen reduction, we assemble a flow cell in which the cathode and anode simultaneously produce H2O2. It shows a Faradaic efficiency of 150% of H2O2 at 1 A cm−2 with a cell voltage of 2.3 V. |
| format | Article |
| id | doaj-art-177ecad6cec54f63996bad7babde830e |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-10-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-177ecad6cec54f63996bad7babde830e2025-08-20T02:17:53ZengNature PortfolioNature Communications2041-17232024-10-0115111010.1038/s41467-024-53134-3Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxideHeng Zhu0Ximei Lv1Yuexu Wu2Wentao Wang3Yuping Wu4Shicheng Yan5Yuhui Chen6State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityKey Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast UniversityCollaborative Innovation Center of Advanced Microstructures, National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Nanjing UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityAbstract Water electro-oxidation to form H2O2 is an important way to produce H2O2 which is widely applied in industry. However, its mechanism is under debate and HO(ads), hydroxyl group adsorbed onto the surface of the electrode, is regarded as an important intermediate. Herein, we study the mechanism of water oxidation to H2O2 at Pt electrode using in-situ Raman spectroscopy and differential electrochemical mass spectroscopy and find peroxide bond mainly originated from the coupling of two CO3 2- via a C2O6 2- intermediate. By quantifying the 18O isotope in the product, we find that 93% of H2O2 was formed via the CO3 2- coupling route and 7% of H2O2 is from OH(ads)-CO3 •− route. The OH(ads)-OH(ads) coupling route has a negligible contribution. The comparison of various electrodes shows that the strong adsorption of CO3(ads) at the electrode surface is essential. Combining with a commercial cathode catalyst to produce H2O2 during oxygen reduction, we assemble a flow cell in which the cathode and anode simultaneously produce H2O2. It shows a Faradaic efficiency of 150% of H2O2 at 1 A cm−2 with a cell voltage of 2.3 V.https://doi.org/10.1038/s41467-024-53134-3 |
| spellingShingle | Heng Zhu Ximei Lv Yuexu Wu Wentao Wang Yuping Wu Shicheng Yan Yuhui Chen Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide Nature Communications |
| title | Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| title_full | Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| title_fullStr | Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| title_full_unstemmed | Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| title_short | Carbonate-carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| title_sort | carbonate carbonate coupling on platinum surface promotes electrochemical water oxidation to hydrogen peroxide |
| url | https://doi.org/10.1038/s41467-024-53134-3 |
| work_keys_str_mv | AT hengzhu carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT ximeilv carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT yuexuwu carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT wentaowang carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT yupingwu carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT shichengyan carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide AT yuhuichen carbonatecarbonatecouplingonplatinumsurfacepromoteselectrochemicalwateroxidationtohydrogenperoxide |