Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis
Electrocatalytic nitrogen reduction reaction (NRR) can realize the green production of ammonia while developing electrocatalysts with high selectivity and ability is still an ongoing challenge. Two-dimensional (2D) graphitic carbon nitride (CN) frameworks can provide abundant hollow sites for stably...
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| Format: | Article |
| Language: | English |
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MDPI AG
2023-05-01
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| Series: | Catalysts |
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| Online Access: | https://www.mdpi.com/2073-4344/13/5/869 |
| _version_ | 1797600705240891392 |
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| author | Shuo Wang Tingting Zhao Likai Yan |
| author_facet | Shuo Wang Tingting Zhao Likai Yan |
| author_sort | Shuo Wang |
| collection | DOAJ |
| description | Electrocatalytic nitrogen reduction reaction (NRR) can realize the green production of ammonia while developing electrocatalysts with high selectivity and ability is still an ongoing challenge. Two-dimensional (2D) graphitic carbon nitride (CN) frameworks can provide abundant hollow sites for stably anchoring several transition metal (TM) atoms to facilitate single-cluster catalysis, promising to overcome the problems of low activity and poor selectivity in the process of ammonia synthesis. Herein, extensive density functional theory (DFT) calculations were performed to investigate the feasibility of six bimetallic triatomic clusters Fe<sub>x</sub>Mo<sub>y</sub> (x = 1, 2; x + y = 3) supported on C<sub>6</sub>N<sub>6</sub>, C<sub>2</sub>N, and N-doped porous graphene (NG) as NRR electrocatalysts. Through a systematic screening strategy, we found that the Fe<sub>2</sub>Mo–NG possesses the highest activity with a limiting potential of –0.36 V through the enzymatic mechanism and could be the promising catalyst for NH<sub>3</sub> synthesis. The Fe<sub>2</sub>Mo moiety in Fe<sub>2</sub>Mo–NG moderately regulates the electron transfer between reaction intermediates and NG, which is ascribed to enhanced performance. This work accelerates the rational design of catalysts in the field of NRR and contributes to broadening the understanding of cluster catalysis. |
| first_indexed | 2024-03-11T03:51:39Z |
| format | Article |
| id | doaj.art-5d295940405e498ca567c64d10b34940 |
| institution | Directory Open Access Journal |
| issn | 2073-4344 |
| language | English |
| last_indexed | 2024-03-11T03:51:39Z |
| publishDate | 2023-05-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Catalysts |
| spelling | doaj.art-5d295940405e498ca567c64d10b349402023-11-18T00:51:26ZengMDPI AGCatalysts2073-43442023-05-0113586910.3390/catal13050869Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia SynthesisShuo Wang0Tingting Zhao1Likai Yan2Institute of Functional Material Chemistry, Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun 130024, ChinaInstitute of Functional Material Chemistry, Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun 130024, ChinaInstitute of Functional Material Chemistry, Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun 130024, ChinaElectrocatalytic nitrogen reduction reaction (NRR) can realize the green production of ammonia while developing electrocatalysts with high selectivity and ability is still an ongoing challenge. Two-dimensional (2D) graphitic carbon nitride (CN) frameworks can provide abundant hollow sites for stably anchoring several transition metal (TM) atoms to facilitate single-cluster catalysis, promising to overcome the problems of low activity and poor selectivity in the process of ammonia synthesis. Herein, extensive density functional theory (DFT) calculations were performed to investigate the feasibility of six bimetallic triatomic clusters Fe<sub>x</sub>Mo<sub>y</sub> (x = 1, 2; x + y = 3) supported on C<sub>6</sub>N<sub>6</sub>, C<sub>2</sub>N, and N-doped porous graphene (NG) as NRR electrocatalysts. Through a systematic screening strategy, we found that the Fe<sub>2</sub>Mo–NG possesses the highest activity with a limiting potential of –0.36 V through the enzymatic mechanism and could be the promising catalyst for NH<sub>3</sub> synthesis. The Fe<sub>2</sub>Mo moiety in Fe<sub>2</sub>Mo–NG moderately regulates the electron transfer between reaction intermediates and NG, which is ascribed to enhanced performance. This work accelerates the rational design of catalysts in the field of NRR and contributes to broadening the understanding of cluster catalysis.https://www.mdpi.com/2073-4344/13/5/869N<sub>2</sub> reduction reactiondensity functional theorysingle-atom catalystcarbon nitride materials |
| spellingShingle | Shuo Wang Tingting Zhao Likai Yan Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis Catalysts N<sub>2</sub> reduction reaction density functional theory single-atom catalyst carbon nitride materials |
| title | Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis |
| title_full | Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis |
| title_fullStr | Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis |
| title_full_unstemmed | Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis |
| title_short | Tailoring of Three-Atom Metal Cluster Catalysts for Ammonia Synthesis |
| title_sort | tailoring of three atom metal cluster catalysts for ammonia synthesis |
| topic | N<sub>2</sub> reduction reaction density functional theory single-atom catalyst carbon nitride materials |
| url | https://www.mdpi.com/2073-4344/13/5/869 |
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