Pt/IrO x enables selective electrochemical C-H chlorination at high current
Abstract Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp 3)-H bond functionalization and low water solubility of such alkanes make it challenging....
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55283-x |
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| author | Bo Wu Ruihu Lu Chao Wu Tenghui Yuan Bin Liu Xi Wang Chenyi Fang Ziyu Mi Surani Bin Dolmanan Weng Weei Tjiu Mingsheng Zhang Bingqing Wang Zainul Aabdin Sui Zhang Yi Hou Bote Zhao Shibo Xi Wan Ru Leow Ziyun Wang Yanwei Lum |
| author_facet | Bo Wu Ruihu Lu Chao Wu Tenghui Yuan Bin Liu Xi Wang Chenyi Fang Ziyu Mi Surani Bin Dolmanan Weng Weei Tjiu Mingsheng Zhang Bingqing Wang Zainul Aabdin Sui Zhang Yi Hou Bote Zhao Shibo Xi Wan Ru Leow Ziyun Wang Yanwei Lum |
| author_sort | Bo Wu |
| collection | DOAJ |
| description | Abstract Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp 3)-H bond functionalization and low water solubility of such alkanes make it challenging. Here we discover that a Pt/IrO x electrocatalyst with optimized Cl binding energy enables selective generation of Cl free radicals for C-H chlorination of alkanes. For instance, we achieve monochlorination of cyclohexane with a current up to 5 A, Faradaic efficiency (FE) up to 95% and stable performance over 100 h in aqueous KCl electrolyte. We further demonstrate that our system can directly utilize concentrated seawater derived from a solar evaporation reverse osmosis process, achieving a FE of 93.8% towards chlorocyclohexane at a current of 1 A. By coupling to a photovoltaic module, we showcase solar-driven production of chlorocyclohexane using concentrated seawater in a membrane electrode assembly cell without any external bias. Our findings constitute a sustainable pathway towards renewable energy driven chemicals manufacture using abundant feedstock at industrially relevant rates. |
| format | Article |
| id | doaj-art-007dcc40feb14e429b94861563fa1bc1 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-007dcc40feb14e429b94861563fa1bc12025-01-05T12:39:45ZengNature PortfolioNature Communications2041-17232025-01-0116111510.1038/s41467-024-55283-xPt/IrO x enables selective electrochemical C-H chlorination at high currentBo Wu0Ruihu Lu1Chao Wu2Tenghui Yuan3Bin Liu4Xi Wang5Chenyi Fang6Ziyu Mi7Surani Bin Dolmanan8Weng Weei Tjiu9Mingsheng Zhang10Bingqing Wang11Zainul Aabdin12Sui Zhang13Yi Hou14Bote Zhao15Shibo Xi16Wan Ru Leow17Ziyun Wang18Yanwei Lum19Department of Chemical and Biomolecular Engineering, National University of SingaporeSchool of Chemical Sciences, The University of AucklandInstitute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR)School of Environment and Energy, South China University of TechnologyDepartment of Chemical and Environmental Engineering, Yale UniversityDepartment of Chemical and Biomolecular Engineering, National University of SingaporeDepartment of Chemical and Biomolecular Engineering, National University of SingaporeInstitute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Department of Chemical and Biomolecular Engineering, National University of SingaporeInstitute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Department of Chemical and Biomolecular Engineering, National University of SingaporeDepartment of Chemical and Biomolecular Engineering, National University of SingaporeSchool of Environment and Energy, South China University of TechnologyInstitute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR)Institute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR)School of Chemical Sciences, The University of AucklandDepartment of Chemical and Biomolecular Engineering, National University of SingaporeAbstract Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp 3)-H bond functionalization and low water solubility of such alkanes make it challenging. Here we discover that a Pt/IrO x electrocatalyst with optimized Cl binding energy enables selective generation of Cl free radicals for C-H chlorination of alkanes. For instance, we achieve monochlorination of cyclohexane with a current up to 5 A, Faradaic efficiency (FE) up to 95% and stable performance over 100 h in aqueous KCl electrolyte. We further demonstrate that our system can directly utilize concentrated seawater derived from a solar evaporation reverse osmosis process, achieving a FE of 93.8% towards chlorocyclohexane at a current of 1 A. By coupling to a photovoltaic module, we showcase solar-driven production of chlorocyclohexane using concentrated seawater in a membrane electrode assembly cell without any external bias. Our findings constitute a sustainable pathway towards renewable energy driven chemicals manufacture using abundant feedstock at industrially relevant rates.https://doi.org/10.1038/s41467-024-55283-x |
| spellingShingle | Bo Wu Ruihu Lu Chao Wu Tenghui Yuan Bin Liu Xi Wang Chenyi Fang Ziyu Mi Surani Bin Dolmanan Weng Weei Tjiu Mingsheng Zhang Bingqing Wang Zainul Aabdin Sui Zhang Yi Hou Bote Zhao Shibo Xi Wan Ru Leow Ziyun Wang Yanwei Lum Pt/IrO x enables selective electrochemical C-H chlorination at high current Nature Communications |
| title | Pt/IrO x enables selective electrochemical C-H chlorination at high current |
| title_full | Pt/IrO x enables selective electrochemical C-H chlorination at high current |
| title_fullStr | Pt/IrO x enables selective electrochemical C-H chlorination at high current |
| title_full_unstemmed | Pt/IrO x enables selective electrochemical C-H chlorination at high current |
| title_short | Pt/IrO x enables selective electrochemical C-H chlorination at high current |
| title_sort | pt iro x enables selective electrochemical c h chlorination at high current |
| url | https://doi.org/10.1038/s41467-024-55283-x |
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