Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis
Abstract The emergence of single-atom catalysts offers exciting prospects for the green production of hydrogen peroxide; however, their optimal local structure and the underlying structure–activity relationships remain unclear. Here we show trace Fe, up to 278 mg/kg and derived from microbial protei...
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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/s41467-024-55041-z |
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| _version_ | 1841559275301765120 |
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| author | Xiaofeng Xiao Zechao Zhuang Shuhu Yin Jiexin Zhu Tao Gan Ruohan Yu Jinsong Wu Xiaochun Tian Yanxia Jiang Dingsheng Wang Feng Zhao |
| author_facet | Xiaofeng Xiao Zechao Zhuang Shuhu Yin Jiexin Zhu Tao Gan Ruohan Yu Jinsong Wu Xiaochun Tian Yanxia Jiang Dingsheng Wang Feng Zhao |
| author_sort | Xiaofeng Xiao |
| collection | DOAJ |
| description | Abstract The emergence of single-atom catalysts offers exciting prospects for the green production of hydrogen peroxide; however, their optimal local structure and the underlying structure–activity relationships remain unclear. Here we show trace Fe, up to 278 mg/kg and derived from microbial protein, serve as precursors to synthesize a variety of Fe single-atom catalysts containing FeN5−x O x (1 ≤ x ≤ 4) moieties through controlled pyrolysis. These moieties resemble the structural features of nonheme Fe-dependent enzymes while being effectively confined on a microbe-derived, electrically conductive carbon support, enabling high-current density electrolysis. A comparative analysis involving catalysts derived from eleven representative microbes reveals that the presence of 0.05 wt% Fe single-atom sites leads to a significant 26% increase in hydrogen peroxide selectivity. Remarkably, the optimal catalyst featuring FeN3O2 sites demonstrates a selectivity of up to 93.7% and generates hydrogen peroxide in a flow cell at an impressive rate of 29.6 mol g−1 h−1 at 200 mA cm−2. This work achieves structural fine-tuning of metal single-atom sites at the trace level and provides topological insights into single-atom catalyst design to achieve cost-efficient hydrogen peroxide production. |
| format | Article |
| id | doaj-art-3cc92944d9d04871b179b5de64654262 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-3cc92944d9d04871b179b5de646542622025-01-05T12:35:50ZengNature PortfolioNature Communications2041-17232024-12-0115111310.1038/s41467-024-55041-zTopological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesisXiaofeng Xiao0Zechao Zhuang1Shuhu Yin2Jiexin Zhu3Tao Gan4Ruohan Yu5Jinsong Wu6Xiaochun Tian7Yanxia Jiang8Dingsheng Wang9Feng Zhao10Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of SciencesDepartment of Chemistry, Tsinghua UniversityCollege of Chemistry and Chemical Engineering, Discipline of Intelligent Instrument and Equipment, Xiamen UniversityState Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of TechnologyShanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of SciencesNanostructure Research Centre, Wuhan University of TechnologyNanostructure Research Centre, Wuhan University of TechnologyKey Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of SciencesCollege of Chemistry and Chemical Engineering, Discipline of Intelligent Instrument and Equipment, Xiamen UniversityDepartment of Chemistry, Tsinghua UniversityKey Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of SciencesAbstract The emergence of single-atom catalysts offers exciting prospects for the green production of hydrogen peroxide; however, their optimal local structure and the underlying structure–activity relationships remain unclear. Here we show trace Fe, up to 278 mg/kg and derived from microbial protein, serve as precursors to synthesize a variety of Fe single-atom catalysts containing FeN5−x O x (1 ≤ x ≤ 4) moieties through controlled pyrolysis. These moieties resemble the structural features of nonheme Fe-dependent enzymes while being effectively confined on a microbe-derived, electrically conductive carbon support, enabling high-current density electrolysis. A comparative analysis involving catalysts derived from eleven representative microbes reveals that the presence of 0.05 wt% Fe single-atom sites leads to a significant 26% increase in hydrogen peroxide selectivity. Remarkably, the optimal catalyst featuring FeN3O2 sites demonstrates a selectivity of up to 93.7% and generates hydrogen peroxide in a flow cell at an impressive rate of 29.6 mol g−1 h−1 at 200 mA cm−2. This work achieves structural fine-tuning of metal single-atom sites at the trace level and provides topological insights into single-atom catalyst design to achieve cost-efficient hydrogen peroxide production.https://doi.org/10.1038/s41467-024-55041-z |
| spellingShingle | Xiaofeng Xiao Zechao Zhuang Shuhu Yin Jiexin Zhu Tao Gan Ruohan Yu Jinsong Wu Xiaochun Tian Yanxia Jiang Dingsheng Wang Feng Zhao Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis Nature Communications |
| title | Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis |
| title_full | Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis |
| title_fullStr | Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis |
| title_full_unstemmed | Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis |
| title_short | Topological transformation of microbial proteins into iron single-atom sites for selective hydrogen peroxide electrosynthesis |
| title_sort | topological transformation of microbial proteins into iron single atom sites for selective hydrogen peroxide electrosynthesis |
| url | https://doi.org/10.1038/s41467-024-55041-z |
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