Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries
Lithium-carbon dioxide (Li-CO2) batteries have received increased attention due to their high energy density and fixing CO2 as a major greenhouse gas. At the same time, there are challenges including low activity of cathode and high overpotential in Li-CO2 batteries. Herein, 45 dual-atom catalysts (...
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Elsevier
2025-01-01
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| Series: | Next Materials |
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| author | Jinhui Zhang Yao Liu Tengwen Yan Guanghui Jin Yajing Shen Jing Xu Dashuai Wang |
| author_facet | Jinhui Zhang Yao Liu Tengwen Yan Guanghui Jin Yajing Shen Jing Xu Dashuai Wang |
| author_sort | Jinhui Zhang |
| collection | DOAJ |
| description | Lithium-carbon dioxide (Li-CO2) batteries have received increased attention due to their high energy density and fixing CO2 as a major greenhouse gas. At the same time, there are challenges including low activity of cathode and high overpotential in Li-CO2 batteries. Herein, 45 dual-atom catalysts (DACs) composed of 9 transition metal (TM) atoms doped in nitrogen-doped graphene (M1M2-N-G, M1, M2 = Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn), as cathode catalysts of Li-CO2 batteries, have been studied by using first-principles calculations. According to the thermodynamic stability of the DACs and the ability of CO2 activation, 25 catalysts candidates were screened out. Then, the reaction activity and selectivity of DACs were evaluated by thermodynamical reaction energy and overpotential. Finally, TiMn-N-G displayed the smallest total electrode overpotential 1.83 V during the pathway of Li2CO3 and CrNi-N-G exhibited the smallest total electrode overpotential 0.08 V during the in Li2C2O4 pathway, respectively, which proved that they possessed better catalytic activity tendency in Li-CO2 batteries. This work provides not only a rational design to identify promising graphene-based catalysts, but also a general screen rule for atomic catalysts in Li-CO2 batteries. |
| format | Article |
| id | doaj-art-ee4fe209dbb749a19e67a4c76bff1990 |
| institution | DOAJ |
| issn | 2949-8228 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Next Materials |
| spelling | doaj-art-ee4fe209dbb749a19e67a4c76bff19902025-08-20T03:02:07ZengElsevierNext Materials2949-82282025-01-01610033410.1016/j.nxmate.2024.100334Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteriesJinhui Zhang0Yao Liu1Tengwen Yan2Guanghui Jin3Yajing Shen4Jing Xu5Dashuai Wang6Institute of Zhejiang University-Quzhou, Quzhou 324000, China; Department of Physics, College of Science, Yanbian University, Yanji 133002, ChinaInstitute of Zhejiang University-Quzhou, Quzhou 324000, China; Department of Physics, College of Science, Yanbian University, Yanji 133002, ChinaInstitute of Zhejiang University-Quzhou, Quzhou 324000, China; Department of Physics, College of Science, Yanbian University, Yanji 133002, ChinaInstitute of Zhejiang University-Quzhou, Quzhou 324000, China; Department of Physics, College of Science, Yanbian University, Yanji 133002, ChinaInstitute of Zhejiang University-Quzhou, Quzhou 324000, China; Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China; Corresponding authors at: Institute of Zhejiang University-Quzhou, Quzhou 324000, China.Department of Physics, College of Science, Yanbian University, Yanji 133002, China; Corresponding author.Institute of Zhejiang University-Quzhou, Quzhou 324000, China; Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China; Corresponding authors at: Institute of Zhejiang University-Quzhou, Quzhou 324000, China.Lithium-carbon dioxide (Li-CO2) batteries have received increased attention due to their high energy density and fixing CO2 as a major greenhouse gas. At the same time, there are challenges including low activity of cathode and high overpotential in Li-CO2 batteries. Herein, 45 dual-atom catalysts (DACs) composed of 9 transition metal (TM) atoms doped in nitrogen-doped graphene (M1M2-N-G, M1, M2 = Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn), as cathode catalysts of Li-CO2 batteries, have been studied by using first-principles calculations. According to the thermodynamic stability of the DACs and the ability of CO2 activation, 25 catalysts candidates were screened out. Then, the reaction activity and selectivity of DACs were evaluated by thermodynamical reaction energy and overpotential. Finally, TiMn-N-G displayed the smallest total electrode overpotential 1.83 V during the pathway of Li2CO3 and CrNi-N-G exhibited the smallest total electrode overpotential 0.08 V during the in Li2C2O4 pathway, respectively, which proved that they possessed better catalytic activity tendency in Li-CO2 batteries. This work provides not only a rational design to identify promising graphene-based catalysts, but also a general screen rule for atomic catalysts in Li-CO2 batteries.http://www.sciencedirect.com/science/article/pii/S2949822824002314DACsLi-CO2 batteriesCathode catalystsCatalytic activity and selectivityFirst principles calculations |
| spellingShingle | Jinhui Zhang Yao Liu Tengwen Yan Guanghui Jin Yajing Shen Jing Xu Dashuai Wang Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries Next Materials DACs Li-CO2 batteries Cathode catalysts Catalytic activity and selectivity First principles calculations |
| title | Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries |
| title_full | Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries |
| title_fullStr | Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries |
| title_full_unstemmed | Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries |
| title_short | Activity evaluation and reaction mechanisms of highly efficient dual-atom transition metal catalysts in Li-CO2 batteries |
| title_sort | activity evaluation and reaction mechanisms of highly efficient dual atom transition metal catalysts in li co2 batteries |
| topic | DACs Li-CO2 batteries Cathode catalysts Catalytic activity and selectivity First principles calculations |
| url | http://www.sciencedirect.com/science/article/pii/S2949822824002314 |
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