Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen
Abstract Discharge of wastewater containing nitrate (NO3 −) disrupts aquatic ecosystems even at low concentrations. However, selective and rapid reduction of NO3 − at low concentration to dinitrogen (N2) is technically challenging. Here, we present an electrified membrane (EM) loaded with Sn pair-at...
Saved in:
| Main Authors: | , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-01-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56102-7 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1832571494313492480 |
|---|---|
| author | Xuanhao Wu Xiaoxiong Wang Yunshuo Wu Huimin Xu Zhe Li Rongrong Hong Kali Rigby Zhongbiao Wu Jae-Hong Kim |
| author_facet | Xuanhao Wu Xiaoxiong Wang Yunshuo Wu Huimin Xu Zhe Li Rongrong Hong Kali Rigby Zhongbiao Wu Jae-Hong Kim |
| author_sort | Xuanhao Wu |
| collection | DOAJ |
| description | Abstract Discharge of wastewater containing nitrate (NO3 −) disrupts aquatic ecosystems even at low concentrations. However, selective and rapid reduction of NO3 − at low concentration to dinitrogen (N2) is technically challenging. Here, we present an electrified membrane (EM) loaded with Sn pair-atom catalysts for highly efficient NO3 − reduction to N2 in a single-pass electrofiltration. The pair-atom design facilitates coupling of adsorbed N intermediates on adjacent Sn atoms to enhance N2 selectivity, which is challenging with conventional fully-isolated single-atom catalyst design. The EM ensures sufficient exposure of the catalysts and intensifies the catalyst interaction with NO3 − through mass transfer enhancement to provide more N intermediates for N2 coupling. We further develop a reduced titanium dioxide EM as the anode to generate free chlorines for fully oxidizing the residual ammonia (<1 mg-N L−1) to N2. The sequential cathode-to-anode electrofiltration realizes near-complete removal of 10 mg-N L−1 NO3 − and ~100% N2 selectivity with a water resident time on the order of seconds. Our findings advance the single-atom catalyst design for NO3 − reduction and provide a practical solution for NO3 − contamination at low concentrations. |
| format | Article |
| id | doaj-art-0c9e175743fe4f1a8f41c37979306e2c |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-0c9e175743fe4f1a8f41c37979306e2c2025-02-02T12:32:08ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-025-56102-7Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogenXuanhao Wu0Xiaoxiong Wang1Yunshuo Wu2Huimin Xu3Zhe Li4Rongrong Hong5Kali Rigby6Zhongbiao Wu7Jae-Hong Kim8Department of Environmental Engineering, Zhejiang UniversityInstitute for Ocean Engineering & Center of Double Helix & Shenzhen Key Laboratory of Advanced Technology for Marine Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua UniversityDepartment of Environmental Engineering, Zhejiang UniversityDepartment of Environmental Engineering, Zhejiang UniversityDepartment of Environmental Engineering, Zhejiang UniversityDepartment of Environmental Engineering, Zhejiang UniversityDepartment of Chemical and Environmental Engineering, Yale UniversityDepartment of Environmental Engineering, Zhejiang UniversityDepartment of Chemical and Environmental Engineering, Yale UniversityAbstract Discharge of wastewater containing nitrate (NO3 −) disrupts aquatic ecosystems even at low concentrations. However, selective and rapid reduction of NO3 − at low concentration to dinitrogen (N2) is technically challenging. Here, we present an electrified membrane (EM) loaded with Sn pair-atom catalysts for highly efficient NO3 − reduction to N2 in a single-pass electrofiltration. The pair-atom design facilitates coupling of adsorbed N intermediates on adjacent Sn atoms to enhance N2 selectivity, which is challenging with conventional fully-isolated single-atom catalyst design. The EM ensures sufficient exposure of the catalysts and intensifies the catalyst interaction with NO3 − through mass transfer enhancement to provide more N intermediates for N2 coupling. We further develop a reduced titanium dioxide EM as the anode to generate free chlorines for fully oxidizing the residual ammonia (<1 mg-N L−1) to N2. The sequential cathode-to-anode electrofiltration realizes near-complete removal of 10 mg-N L−1 NO3 − and ~100% N2 selectivity with a water resident time on the order of seconds. Our findings advance the single-atom catalyst design for NO3 − reduction and provide a practical solution for NO3 − contamination at low concentrations.https://doi.org/10.1038/s41467-025-56102-7 |
| spellingShingle | Xuanhao Wu Xiaoxiong Wang Yunshuo Wu Huimin Xu Zhe Li Rongrong Hong Kali Rigby Zhongbiao Wu Jae-Hong Kim Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen Nature Communications |
| title | Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen |
| title_full | Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen |
| title_fullStr | Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen |
| title_full_unstemmed | Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen |
| title_short | Bilayer electrified-membrane with pair-atom tin catalysts for near-complete conversion of low concentration nitrate to dinitrogen |
| title_sort | bilayer electrified membrane with pair atom tin catalysts for near complete conversion of low concentration nitrate to dinitrogen |
| url | https://doi.org/10.1038/s41467-025-56102-7 |
| work_keys_str_mv | AT xuanhaowu bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT xiaoxiongwang bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT yunshuowu bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT huiminxu bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT zheli bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT rongronghong bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT kalirigby bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT zhongbiaowu bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen AT jaehongkim bilayerelectrifiedmembranewithpairatomtincatalystsfornearcompleteconversionoflowconcentrationnitratetodinitrogen |