Designer topological-single-atom catalysts with site-specific selectivity
Abstract Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio mo...
Saved in:
| Main Authors: | , , , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-01-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-55838-6 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1841544437668249600 |
|---|---|
| author | Weibin Chen Menghui Bao Fanqi Meng Bingbing Ma Long Feng Xuan Zhang Zanlin Qiu Song Gao Ruiqin Zhong Shibo Xi Xiao Hai Jiong Lu Ruqiang Zou |
| author_facet | Weibin Chen Menghui Bao Fanqi Meng Bingbing Ma Long Feng Xuan Zhang Zanlin Qiu Song Gao Ruiqin Zhong Shibo Xi Xiao Hai Jiong Lu Ruqiang Zou |
| author_sort | Weibin Chen |
| collection | DOAJ |
| description | Abstract Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio molecular dynamics (AIMD) calculations, where metal single atoms are arranged in asymmetric configurations that electronic shield topologically misorients d orbitals, minimizing unwanted interactions between reactants and the support surface. Mn1/CeO2 catalysts, synthesized via a charge-transfer-driven approach, demonstrate superior catalytic activity and selectivity for NO x removal. A life-cycle assessment (LCA) reveals that Mn1/CeO2 significantly reduces environmental impact compared to traditional V-W-Ti catalysts. Through in-situ spectroscopic characterizations combined with DFT calculations, we elucidate detailed reaction mechanisms. This study establishes T-SACs as a promising class of catalysts, offering a systematic framework to address catalytic challenges by defining site characteristics. The concept highlights their potential for advancing selective catalytic processes and promoting sustainable technologies. |
| format | Article |
| id | doaj-art-68f962583e064d069f58f6006ebbcbd4 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-68f962583e064d069f58f6006ebbcbd42025-01-12T12:31:16ZengNature PortfolioNature Communications2041-17232025-01-0116111510.1038/s41467-025-55838-6Designer topological-single-atom catalysts with site-specific selectivityWeibin Chen0Menghui Bao1Fanqi Meng2Bingbing Ma3Long Feng4Xuan Zhang5Zanlin Qiu6Song Gao7Ruiqin Zhong8Shibo Xi9Xiao Hai10Jiong Lu11Ruqiang Zou12School of Materials Science and Engineering, Peking UniversityState Key Laboratory of Heavy Oil Processing, China University of PetroleumSchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversityState Key Laboratory of Heavy Oil Processing, China University of PetroleumSchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversityState Key Laboratory of Heavy Oil Processing, China University of PetroleumInstitute of Sustainability for Chemicals, Energy and Environment (ISCE2), Agency for Science, Technology and Research (A*STAR)School of Materials Science and Engineering, Peking UniversityDepartment of Chemistry, National University of SingaporeSchool of Materials Science and Engineering, Peking UniversityAbstract Designing catalysts with well-defined, identical sites that achieve site-specific selectivity, and activity remains a significant challenge. In this work, we introduce a design principle of topological-single-atom catalysts (T-SACs) guided by density functional theory (DFT) and Ab initio molecular dynamics (AIMD) calculations, where metal single atoms are arranged in asymmetric configurations that electronic shield topologically misorients d orbitals, minimizing unwanted interactions between reactants and the support surface. Mn1/CeO2 catalysts, synthesized via a charge-transfer-driven approach, demonstrate superior catalytic activity and selectivity for NO x removal. A life-cycle assessment (LCA) reveals that Mn1/CeO2 significantly reduces environmental impact compared to traditional V-W-Ti catalysts. Through in-situ spectroscopic characterizations combined with DFT calculations, we elucidate detailed reaction mechanisms. This study establishes T-SACs as a promising class of catalysts, offering a systematic framework to address catalytic challenges by defining site characteristics. The concept highlights their potential for advancing selective catalytic processes and promoting sustainable technologies.https://doi.org/10.1038/s41467-025-55838-6 |
| spellingShingle | Weibin Chen Menghui Bao Fanqi Meng Bingbing Ma Long Feng Xuan Zhang Zanlin Qiu Song Gao Ruiqin Zhong Shibo Xi Xiao Hai Jiong Lu Ruqiang Zou Designer topological-single-atom catalysts with site-specific selectivity Nature Communications |
| title | Designer topological-single-atom catalysts with site-specific selectivity |
| title_full | Designer topological-single-atom catalysts with site-specific selectivity |
| title_fullStr | Designer topological-single-atom catalysts with site-specific selectivity |
| title_full_unstemmed | Designer topological-single-atom catalysts with site-specific selectivity |
| title_short | Designer topological-single-atom catalysts with site-specific selectivity |
| title_sort | designer topological single atom catalysts with site specific selectivity |
| url | https://doi.org/10.1038/s41467-025-55838-6 |
| work_keys_str_mv | AT weibinchen designertopologicalsingleatomcatalystswithsitespecificselectivity AT menghuibao designertopologicalsingleatomcatalystswithsitespecificselectivity AT fanqimeng designertopologicalsingleatomcatalystswithsitespecificselectivity AT bingbingma designertopologicalsingleatomcatalystswithsitespecificselectivity AT longfeng designertopologicalsingleatomcatalystswithsitespecificselectivity AT xuanzhang designertopologicalsingleatomcatalystswithsitespecificselectivity AT zanlinqiu designertopologicalsingleatomcatalystswithsitespecificselectivity AT songgao designertopologicalsingleatomcatalystswithsitespecificselectivity AT ruiqinzhong designertopologicalsingleatomcatalystswithsitespecificselectivity AT shiboxi designertopologicalsingleatomcatalystswithsitespecificselectivity AT xiaohai designertopologicalsingleatomcatalystswithsitespecificselectivity AT jionglu designertopologicalsingleatomcatalystswithsitespecificselectivity AT ruqiangzou designertopologicalsingleatomcatalystswithsitespecificselectivity |