Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis
Ammonia (NH<sub>3</sub>) synthesis is one of the most important catalytic reactions in energy and chemical fertilizer production, which is of great significance to the sustainable development of society and the economy. The electrochemical nitrogen reduction reaction (eNRR), especially w...
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| Format: | Article |
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MDPI AG
2023-05-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/28/10/4003 |
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| author | Xiaoli Yang Ping An Ruiying Wang Jianfeng Jia |
| author_facet | Xiaoli Yang Ping An Ruiying Wang Jianfeng Jia |
| author_sort | Xiaoli Yang |
| collection | DOAJ |
| description | Ammonia (NH<sub>3</sub>) synthesis is one of the most important catalytic reactions in energy and chemical fertilizer production, which is of great significance to the sustainable development of society and the economy. The electrochemical nitrogen reduction reaction (eNRR), especially when driven by renewable energy, is generally regarded as an energy-efficient and sustainable process to synthesize NH<sub>3</sub> in ambient conditions. However, the performance of the electrocatalyst is far below expectations, with the lack of a high-efficiency catalyst being the main obstacle. Herein, by means of comprehensive spin-polarized density functional theory (DFT) computations, the catalytic performance of MoTM/C<sub>2</sub>N (TM = 3d transition metal) for use in eNRR was systematically evaluated. Among the results, MoFe/C<sub>2</sub>N can be considered the most promising catalyst due to its having the lowest limiting potential (−0.26 V) and high selectivity in the context of eNRR. Compared with its homonuclear counterparts, MoMo/C<sub>2</sub>N and FeFe/C<sub>2</sub>N, MoFe/C<sub>2</sub>N can balance the first protonation step and the sixth protonation step synergistically, showing outstanding activity regarding eNRR. Our work not only opens a new door to advancing sustainable NH<sub>3</sub> production by tailoring the active sites of heteronuclear diatom catalysts but also promotes the design and production of novel low-cost and efficient nanocatalysts. |
| first_indexed | 2024-03-11T03:27:07Z |
| format | Article |
| id | doaj.art-207b32014f7b4f669be4c2a16c50ea68 |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-11T03:27:07Z |
| publishDate | 2023-05-01 |
| publisher | MDPI AG |
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| series | Molecules |
| spelling | doaj.art-207b32014f7b4f669be4c2a16c50ea682023-11-18T02:37:53ZengMDPI AGMolecules1420-30492023-05-012810400310.3390/molecules28104003Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia SynthesisXiaoli Yang0Ping An1Ruiying Wang2Jianfeng Jia3Key Laboratory of Magnetic Molecules and Magnetic Information Materials (Ministry of Education), School of Chemistry and Material Science, Shanxi Normal University, Taiyuan 030031, ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials (Ministry of Education), School of Chemistry and Material Science, Shanxi Normal University, Taiyuan 030031, ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials (Ministry of Education), School of Chemistry and Material Science, Shanxi Normal University, Taiyuan 030031, ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials (Ministry of Education), School of Chemistry and Material Science, Shanxi Normal University, Taiyuan 030031, ChinaAmmonia (NH<sub>3</sub>) synthesis is one of the most important catalytic reactions in energy and chemical fertilizer production, which is of great significance to the sustainable development of society and the economy. The electrochemical nitrogen reduction reaction (eNRR), especially when driven by renewable energy, is generally regarded as an energy-efficient and sustainable process to synthesize NH<sub>3</sub> in ambient conditions. However, the performance of the electrocatalyst is far below expectations, with the lack of a high-efficiency catalyst being the main obstacle. Herein, by means of comprehensive spin-polarized density functional theory (DFT) computations, the catalytic performance of MoTM/C<sub>2</sub>N (TM = 3d transition metal) for use in eNRR was systematically evaluated. Among the results, MoFe/C<sub>2</sub>N can be considered the most promising catalyst due to its having the lowest limiting potential (−0.26 V) and high selectivity in the context of eNRR. Compared with its homonuclear counterparts, MoMo/C<sub>2</sub>N and FeFe/C<sub>2</sub>N, MoFe/C<sub>2</sub>N can balance the first protonation step and the sixth protonation step synergistically, showing outstanding activity regarding eNRR. Our work not only opens a new door to advancing sustainable NH<sub>3</sub> production by tailoring the active sites of heteronuclear diatom catalysts but also promotes the design and production of novel low-cost and efficient nanocatalysts.https://www.mdpi.com/1420-3049/28/10/4003electrochemical ammonia synthesisheteronuclear diatom catalystsdensity functional theory |
| spellingShingle | Xiaoli Yang Ping An Ruiying Wang Jianfeng Jia Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis Molecules electrochemical ammonia synthesis heteronuclear diatom catalysts density functional theory |
| title | Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis |
| title_full | Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis |
| title_fullStr | Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis |
| title_full_unstemmed | Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis |
| title_short | Tuning the Site-to-Site Interaction of Heteronuclear Diatom Catalysts MoTM/C<sub>2</sub>N (TM = 3d Transition Metal) for Electrochemical Ammonia Synthesis |
| title_sort | tuning the site to site interaction of heteronuclear diatom catalysts motm c sub 2 sub n tm 3d transition metal for electrochemical ammonia synthesis |
| topic | electrochemical ammonia synthesis heteronuclear diatom catalysts density functional theory |
| url | https://www.mdpi.com/1420-3049/28/10/4003 |
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