Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production
Abstract Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and dur...
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-07-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-40118-y |
| _version_ | 1797774112993574912 |
|---|---|
| author | Wei Peng Jiaxin Liu Xiaoqing Liu Liqun Wang Lichang Yin Haotian Tan Feng Hou Ji Liang |
| author_facet | Wei Peng Jiaxin Liu Xiaoqing Liu Liqun Wang Lichang Yin Haotian Tan Feng Hou Ji Liang |
| author_sort | Wei Peng |
| collection | DOAJ |
| description | Abstract Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e− oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H2O2 production. Consequently, the H2O2 yield approaches 30 mol g−1 h−1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L−1. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e− oxygen reduction. |
| first_indexed | 2024-03-12T22:15:20Z |
| format | Article |
| id | doaj.art-cf867f91c56640898be0e32435b58591 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-12T22:15:20Z |
| publishDate | 2023-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-cf867f91c56640898be0e32435b585912023-07-23T11:19:42ZengNature PortfolioNature Communications2041-17232023-07-0114111110.1038/s41467-023-40118-yFacilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide productionWei Peng0Jiaxin Liu1Xiaoqing Liu2Liqun Wang3Lichang Yin4Haotian Tan5Feng Hou6Ji Liang7Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityApplied Physics Department, College of Physics and Materials Science, Tianjin Normal UniversityShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of SciencesKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityKey Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin UniversityAbstract Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e− oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H2O2 production. Consequently, the H2O2 yield approaches 30 mol g−1 h−1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L−1. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e− oxygen reduction.https://doi.org/10.1038/s41467-023-40118-y |
| spellingShingle | Wei Peng Jiaxin Liu Xiaoqing Liu Liqun Wang Lichang Yin Haotian Tan Feng Hou Ji Liang Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production Nature Communications |
| title | Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| title_full | Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| title_fullStr | Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| title_full_unstemmed | Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| title_short | Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| title_sort | facilitating two electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production |
| url | https://doi.org/10.1038/s41467-023-40118-y |
| work_keys_str_mv | AT weipeng facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT jiaxinliu facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT xiaoqingliu facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT liqunwang facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT lichangyin facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT haotiantan facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT fenghou facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction AT jiliang facilitatingtwoelectronoxygenreductionwithpyrrolicnitrogensitesforelectrochemicalhydrogenperoxideproduction |