Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis
Abstract The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H2O2 electrosynthesis community. However, it remains perplexing that electrocatalysts and assembled GDE frequently ex...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-12-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55091-3 |
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| author | Lele Cui Bin Chen Dongxu Chen Chen He Yi Liu Hongyi Zhang Jian Qiu Le Liu Wenheng Jing Zhenghua Zhang |
| author_facet | Lele Cui Bin Chen Dongxu Chen Chen He Yi Liu Hongyi Zhang Jian Qiu Le Liu Wenheng Jing Zhenghua Zhang |
| author_sort | Lele Cui |
| collection | DOAJ |
| description | Abstract The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H2O2 electrosynthesis community. However, it remains perplexing that electrocatalysts and assembled GDE frequently exhibit substantial discrepancies in H2O2 selectivity during bulk electrolysis. Here, we elucidate the pivotal role of mass transfer behavior of key species (including reactants and products) beyond the intrinsic properties of the electrocatalyst in dictating electrode-scale H2O2 selectivity. This tendency becomes more pronounced in high reaction rate (current density) regimes where transport limitations are intensified. By utilizing diffusion-related parameters (DRP) of GDEs (i.e., wettability and catalyst layer thickness) as probe factors, we employ both short- and long-term electrolysis in conjunction with in-situ electrochemical reflection-absorption imaging and theoretical calculations to thoroughly investigate the impact of DRP and DRP-controlled local microenvironments on O2 and H2O2 mass transfer. The mechanistic origins of diffusion-dependent conversion selectivity at the electrode scale are unveiled accordingly. The fundamental insights gained from this study underscore the necessity of architectural innovations for mainstream hydrophobic GDEs that can synchronously optimize mass transfer of reactants and products, paving the way for next-generation GDEs in gas-consuming electroreduction scenarios. |
| format | Article |
| id | doaj-art-60af592c4e6145f1984c2125d88cfeaf |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-60af592c4e6145f1984c2125d88cfeaf2025-08-20T02:30:54ZengNature PortfolioNature Communications2041-17232024-12-0115111510.1038/s41467-024-55091-3Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesisLele Cui0Bin Chen1Dongxu Chen2Chen He3Yi Liu4Hongyi Zhang5Jian Qiu6Le Liu7Wenheng Jing8Zhenghua Zhang9Membrane & Nanotechnology-Enabled Water Treatment Center, Guangdong Provincial Engineering Research Centre for Urban Water Recycling and Environmental Safety, Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityInstitute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityMembrane & Nanotechnology-Enabled Water Treatment Center, Guangdong Provincial Engineering Research Centre for Urban Water Recycling and Environmental Safety, Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityMembrane & Nanotechnology-Enabled Water Treatment Center, Guangdong Provincial Engineering Research Centre for Urban Water Recycling and Environmental Safety, Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityInstitute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityState Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech UniversityMembrane & Nanotechnology-Enabled Water Treatment Center, Guangdong Provincial Engineering Research Centre for Urban Water Recycling and Environmental Safety, Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityAbstract The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H2O2 electrosynthesis community. However, it remains perplexing that electrocatalysts and assembled GDE frequently exhibit substantial discrepancies in H2O2 selectivity during bulk electrolysis. Here, we elucidate the pivotal role of mass transfer behavior of key species (including reactants and products) beyond the intrinsic properties of the electrocatalyst in dictating electrode-scale H2O2 selectivity. This tendency becomes more pronounced in high reaction rate (current density) regimes where transport limitations are intensified. By utilizing diffusion-related parameters (DRP) of GDEs (i.e., wettability and catalyst layer thickness) as probe factors, we employ both short- and long-term electrolysis in conjunction with in-situ electrochemical reflection-absorption imaging and theoretical calculations to thoroughly investigate the impact of DRP and DRP-controlled local microenvironments on O2 and H2O2 mass transfer. The mechanistic origins of diffusion-dependent conversion selectivity at the electrode scale are unveiled accordingly. The fundamental insights gained from this study underscore the necessity of architectural innovations for mainstream hydrophobic GDEs that can synchronously optimize mass transfer of reactants and products, paving the way for next-generation GDEs in gas-consuming electroreduction scenarios.https://doi.org/10.1038/s41467-024-55091-3 |
| spellingShingle | Lele Cui Bin Chen Dongxu Chen Chen He Yi Liu Hongyi Zhang Jian Qiu Le Liu Wenheng Jing Zhenghua Zhang Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis Nature Communications |
| title | Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis |
| title_full | Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis |
| title_fullStr | Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis |
| title_full_unstemmed | Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis |
| title_short | Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis |
| title_sort | species mass transfer governs the selectivity of gas diffusion electrodes toward h2o2 electrosynthesis |
| url | https://doi.org/10.1038/s41467-024-55091-3 |
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