CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting
Abstract Optimizing the electronic structure with increasing intrinsic stability is a usual method to enhance the catalysts’ performance. Herein, a series of cerium dioxide (CeO2−δ) based solid solution materials is synthesized via substituting Ce atoms with transition metal (Co, Cu, Ni, etc.), in w...
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Wiley
2025-01-01
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| Online Access: | https://doi.org/10.1002/advs.202411845 |
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| author | Gege Su Yichao Hou Jie Yin Jiayi Yang Zhenglong Li Xin Du Xin Zhang Pinxian Xi Chun‐Hua Yan |
| author_facet | Gege Su Yichao Hou Jie Yin Jiayi Yang Zhenglong Li Xin Du Xin Zhang Pinxian Xi Chun‐Hua Yan |
| author_sort | Gege Su |
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| description | Abstract Optimizing the electronic structure with increasing intrinsic stability is a usual method to enhance the catalysts’ performance. Herein, a series of cerium dioxide (CeO2−δ) based solid solution materials is synthesized via substituting Ce atoms with transition metal (Co, Cu, Ni, etc.), in which Co0.07Ce0.93O2−δ shows optimized band structure because of electron transition in the reaction, namely Co3+ (3d64s0) + Ce3+ (4f15d 06s0) → Co2+ (3d74s0) + Ce4+ (4f05d06s0), with more stable electronic configuration. The in situ Raman spectra show a stable F2g peak at ≈452 cm−1 of Co0.07Ce0.93O2−δ, while the F2g peak in CeO2−δ almost disappeared during HER progress, demonstrating the charge distribution of *H adsorbed on Co0.07Ce0.93O2−δ is more stable than *H adsorbed on CeO2−δ. Density functional theory calculations reveal that Co0.07Ce0.93O2−δ solid solution increases protonation capacity and favors for formation of *H in alkaline media. General guidelines are formulated for optimizing adsorption capacity and the volcano plot demonstrates the excellent catalytic performance of Co0.07Ce0.93O2−δ solid solution. The alkaline anion exchange membrane water electrolysis based on Co0.07Ce0.93O2−δ/NiFe LDH realizes a current density of 1000 mA cm−2 at ≈1.86 V in alkaline seawater at 80 °C and exhibits long‐term stability for 450 h. |
| format | Article |
| id | doaj-art-8c6eace8d0bb4ff896ba11a18fe217ae |
| institution | Kabale University |
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| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
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| series | Advanced Science |
| spelling | doaj-art-8c6eace8d0bb4ff896ba11a18fe217ae2025-01-29T09:50:18ZengWileyAdvanced Science2198-38442025-01-01124n/an/a10.1002/advs.202411845CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water SplittingGege Su0Yichao Hou1Jie Yin2Jiayi Yang3Zhenglong Li4Xin Du5Xin Zhang6Pinxian Xi7Chun‐Hua Yan8State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaCollege of Chemistry Zhengzhou University Zhengzhou 450001 ChinaSchool of Nuclear Science and Technology Lanzhou University Lanzhou 730000 ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaState Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 P. R. ChinaAbstract Optimizing the electronic structure with increasing intrinsic stability is a usual method to enhance the catalysts’ performance. Herein, a series of cerium dioxide (CeO2−δ) based solid solution materials is synthesized via substituting Ce atoms with transition metal (Co, Cu, Ni, etc.), in which Co0.07Ce0.93O2−δ shows optimized band structure because of electron transition in the reaction, namely Co3+ (3d64s0) + Ce3+ (4f15d 06s0) → Co2+ (3d74s0) + Ce4+ (4f05d06s0), with more stable electronic configuration. The in situ Raman spectra show a stable F2g peak at ≈452 cm−1 of Co0.07Ce0.93O2−δ, while the F2g peak in CeO2−δ almost disappeared during HER progress, demonstrating the charge distribution of *H adsorbed on Co0.07Ce0.93O2−δ is more stable than *H adsorbed on CeO2−δ. Density functional theory calculations reveal that Co0.07Ce0.93O2−δ solid solution increases protonation capacity and favors for formation of *H in alkaline media. General guidelines are formulated for optimizing adsorption capacity and the volcano plot demonstrates the excellent catalytic performance of Co0.07Ce0.93O2−δ solid solution. The alkaline anion exchange membrane water electrolysis based on Co0.07Ce0.93O2−δ/NiFe LDH realizes a current density of 1000 mA cm−2 at ≈1.86 V in alkaline seawater at 80 °C and exhibits long‐term stability for 450 h.https://doi.org/10.1002/advs.202411845alkaline water splittingCeO2−δelectronic structuresHERsolid solutions |
| spellingShingle | Gege Su Yichao Hou Jie Yin Jiayi Yang Zhenglong Li Xin Du Xin Zhang Pinxian Xi Chun‐Hua Yan CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting Advanced Science alkaline water splitting CeO2−δ electronic structures HER solid solutions |
| title | CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting |
| title_full | CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting |
| title_fullStr | CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting |
| title_full_unstemmed | CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting |
| title_short | CeO2−δ as Electron Donor in Co0.07Ce0.93O2−δ Solid Solution Boosts Alkaline Water Splitting |
| title_sort | ceo2 δ as electron donor in co0 07ce0 93o2 δ solid solution boosts alkaline water splitting |
| topic | alkaline water splitting CeO2−δ electronic structures HER solid solutions |
| url | https://doi.org/10.1002/advs.202411845 |
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