High current density electroreduction of CO2 into formate with tin oxide nanospheres
Abstract In this study, we demonstrate three-dimensional (3D) hollow nanosphere electrocatalysts for CO2 conversion into formate with excellent H-Cell performance and industrially-relevant current density in a 25 cm2 membrane electrode assembly electrolyzer device. Varying calcination temperature ma...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2022-05-01
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| Series: | Scientific Reports |
| Online Access: | https://doi.org/10.1038/s41598-022-11890-6 |
| _version_ | 1818240649804120064 |
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| author | Thuy-Duong Nguyen-Phan Leiming Hu Bret H. Howard Wenqian Xu Eli Stavitski Denis Leshchev August Rothenberger Kenneth C. Neyerlin Douglas R. Kauffman |
| author_facet | Thuy-Duong Nguyen-Phan Leiming Hu Bret H. Howard Wenqian Xu Eli Stavitski Denis Leshchev August Rothenberger Kenneth C. Neyerlin Douglas R. Kauffman |
| author_sort | Thuy-Duong Nguyen-Phan |
| collection | DOAJ |
| description | Abstract In this study, we demonstrate three-dimensional (3D) hollow nanosphere electrocatalysts for CO2 conversion into formate with excellent H-Cell performance and industrially-relevant current density in a 25 cm2 membrane electrode assembly electrolyzer device. Varying calcination temperature maximized formate production via optimizing the crystallinity and particle size of the constituent SnO2 nanoparticles. The best performing SnO2 nanosphere catalysts contained ~ 7.5 nm nanocrystals and produced 71–81% formate Faradaic efficiency (FE) between −0.9 V and −1.3 V vs. the reversible hydrogen electrode (RHE) at a maximum formate partial current density of 73 ± 2 mA cmgeo −2 at −1.3 V vs. RHE. The higher performance of nanosphere catalysts over SnO2 nanoparticles and commercially-available catalyst could be ascribed to their initial structure providing higher electrochemical surface area and preventing extensive nanocrystal growth during CO2 reduction. Our results are among the highest performance reported for SnO2 electrocatalysts in aqueous H-cells. We observed an average 68 ± 8% FE over 35 h of operation with multiple on/off cycles. In situ Raman and time-dependent X-ray diffraction measurements identified metallic Sn as electrocatalytic active sites during long-term operation. Further evaluation in a 25 cm2 electrolyzer cell demonstrated impressive performance with a sustained current density of 500 mA cmgeo −2 and an average 75 ± 6% formate FE over 24 h of operation. Our results provide additional design concepts for boosting the performance of formate-producing catalysts. |
| first_indexed | 2024-12-12T13:16:48Z |
| format | Article |
| id | doaj.art-668b67c3a6544e94aa45c0402ead0243 |
| institution | Directory Open Access Journal |
| issn | 2045-2322 |
| language | English |
| last_indexed | 2024-12-12T13:16:48Z |
| publishDate | 2022-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj.art-668b67c3a6544e94aa45c0402ead02432022-12-22T00:23:24ZengNature PortfolioScientific Reports2045-23222022-05-0112111010.1038/s41598-022-11890-6High current density electroreduction of CO2 into formate with tin oxide nanospheresThuy-Duong Nguyen-Phan0Leiming Hu1Bret H. Howard2Wenqian Xu3Eli Stavitski4Denis Leshchev5August Rothenberger6Kenneth C. Neyerlin7Douglas R. Kauffman8National Energy Technology LaboratoryNational Renewable Energy LaboratoryNational Energy Technology LaboratoryX-Ray Science Division, Advanced Photon Source, Argonne National LaboratoryPhoton Sciences Division, National Synchrotron Light Source II, Brookhaven National LaboratoryPhoton Sciences Division, National Synchrotron Light Source II, Brookhaven National LaboratoryNational Energy Technology LaboratoryNational Renewable Energy LaboratoryNational Energy Technology LaboratoryAbstract In this study, we demonstrate three-dimensional (3D) hollow nanosphere electrocatalysts for CO2 conversion into formate with excellent H-Cell performance and industrially-relevant current density in a 25 cm2 membrane electrode assembly electrolyzer device. Varying calcination temperature maximized formate production via optimizing the crystallinity and particle size of the constituent SnO2 nanoparticles. The best performing SnO2 nanosphere catalysts contained ~ 7.5 nm nanocrystals and produced 71–81% formate Faradaic efficiency (FE) between −0.9 V and −1.3 V vs. the reversible hydrogen electrode (RHE) at a maximum formate partial current density of 73 ± 2 mA cmgeo −2 at −1.3 V vs. RHE. The higher performance of nanosphere catalysts over SnO2 nanoparticles and commercially-available catalyst could be ascribed to their initial structure providing higher electrochemical surface area and preventing extensive nanocrystal growth during CO2 reduction. Our results are among the highest performance reported for SnO2 electrocatalysts in aqueous H-cells. We observed an average 68 ± 8% FE over 35 h of operation with multiple on/off cycles. In situ Raman and time-dependent X-ray diffraction measurements identified metallic Sn as electrocatalytic active sites during long-term operation. Further evaluation in a 25 cm2 electrolyzer cell demonstrated impressive performance with a sustained current density of 500 mA cmgeo −2 and an average 75 ± 6% formate FE over 24 h of operation. Our results provide additional design concepts for boosting the performance of formate-producing catalysts.https://doi.org/10.1038/s41598-022-11890-6 |
| spellingShingle | Thuy-Duong Nguyen-Phan Leiming Hu Bret H. Howard Wenqian Xu Eli Stavitski Denis Leshchev August Rothenberger Kenneth C. Neyerlin Douglas R. Kauffman High current density electroreduction of CO2 into formate with tin oxide nanospheres Scientific Reports |
| title | High current density electroreduction of CO2 into formate with tin oxide nanospheres |
| title_full | High current density electroreduction of CO2 into formate with tin oxide nanospheres |
| title_fullStr | High current density electroreduction of CO2 into formate with tin oxide nanospheres |
| title_full_unstemmed | High current density electroreduction of CO2 into formate with tin oxide nanospheres |
| title_short | High current density electroreduction of CO2 into formate with tin oxide nanospheres |
| title_sort | high current density electroreduction of co2 into formate with tin oxide nanospheres |
| url | https://doi.org/10.1038/s41598-022-11890-6 |
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