Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction
Abstract Atomic‐level catalysts are extensively applied in heterogeneous catalysis fields. However, it is a general but ineluctable issue that active metal atoms may migrate, aggregate, deactivate, or leach during reaction processes, suppressing their catalytic performances. Designing superior intri...
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Wiley
2025-07-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202501393 |
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| author | Pei‐Hua Li Yuan‐Fan Yang Zong‐Yin Song Bo Liang Yong‐Huan Zhao Xin Cai Zi‐Hao Liu Jing‐Yi Lin Meng Yang Xiangyu Xiao Jing Zhang Wen‐Qing Liu Xing‐Jiu Huang |
| author_facet | Pei‐Hua Li Yuan‐Fan Yang Zong‐Yin Song Bo Liang Yong‐Huan Zhao Xin Cai Zi‐Hao Liu Jing‐Yi Lin Meng Yang Xiangyu Xiao Jing Zhang Wen‐Qing Liu Xing‐Jiu Huang |
| author_sort | Pei‐Hua Li |
| collection | DOAJ |
| description | Abstract Atomic‐level catalysts are extensively applied in heterogeneous catalysis fields. However, it is a general but ineluctable issue that active metal atoms may migrate, aggregate, deactivate, or leach during reaction processes, suppressing their catalytic performances. Designing superior intrinsic‐structural stability of atomic‐level catalysts with high activity and revealing their dynamic structure evolution is vital for their wide applications in complex reactions or harsh conditions. Herein, high‐stable Pd─Cu dual‐atom catalysts with PdN3─CuN3 coordination structure are engineered via strong chelation of Cu2+‐ions with electron pairs from palladium‐source, achieving the highest turnover frequency under the lowest overpotential for Cr(VI) electrocatalytic reduction detection in strong‐acid electrolytes. In situ X‐ray absorption fine structure spectra reveal dynamic “spring‐effect” of Cu─Pd and Cu─N bonds that are reversibly stretched with potential changes and can be recovered at 0.6 V for regeneration. The modulated electron‐orbit coupling effect of Pd─Cu pairs prevents Cu‐atoms from aggregating as metallic nanoparticles. Pd─Cu dual‐atoms interact with two O atoms of H2CrO4, forming stable bridge configurations and transferring electrons to promote Cr─O bond dissociation, which prominently decreases reaction energy barriers. This work provides a feasible route to boost the stability and robustness of metal single‐atoms that are easily affected by reaction conditions for sustainable catalytic applications. |
| format | Article |
| id | doaj-art-a55fa08b0cfb491c933f6db991afe554 |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-a55fa08b0cfb491c933f6db991afe5542025-08-20T03:32:37ZengWileyAdvanced Science2198-38442025-07-011228n/an/a10.1002/advs.202501393Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic ReductionPei‐Hua Li0Yuan‐Fan Yang1Zong‐Yin Song2Bo Liang3Yong‐Huan Zhao4Xin Cai5Zi‐Hao Liu6Jing‐Yi Lin7Meng Yang8Xiangyu Xiao9Jing Zhang10Wen‐Qing Liu11Xing‐Jiu Huang12Institute of Environment Hefei Comprehensive National Science Center Hefei 230088 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaKey Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS, Chinese Academy of Sciences Hefei 230031 P. R. ChinaInstitute of Environment Hefei Comprehensive National Science Center Hefei 230088 P. R. ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE) School of Environmental and Chemical Engineering Shanghai University Shanghai 200444 P. R. ChinaBeijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. ChinaInstitute of Environment Hefei Comprehensive National Science Center Hefei 230088 P. R. ChinaInstitute of Environment Hefei Comprehensive National Science Center Hefei 230088 P. R. ChinaAbstract Atomic‐level catalysts are extensively applied in heterogeneous catalysis fields. However, it is a general but ineluctable issue that active metal atoms may migrate, aggregate, deactivate, or leach during reaction processes, suppressing their catalytic performances. Designing superior intrinsic‐structural stability of atomic‐level catalysts with high activity and revealing their dynamic structure evolution is vital for their wide applications in complex reactions or harsh conditions. Herein, high‐stable Pd─Cu dual‐atom catalysts with PdN3─CuN3 coordination structure are engineered via strong chelation of Cu2+‐ions with electron pairs from palladium‐source, achieving the highest turnover frequency under the lowest overpotential for Cr(VI) electrocatalytic reduction detection in strong‐acid electrolytes. In situ X‐ray absorption fine structure spectra reveal dynamic “spring‐effect” of Cu─Pd and Cu─N bonds that are reversibly stretched with potential changes and can be recovered at 0.6 V for regeneration. The modulated electron‐orbit coupling effect of Pd─Cu pairs prevents Cu‐atoms from aggregating as metallic nanoparticles. Pd─Cu dual‐atoms interact with two O atoms of H2CrO4, forming stable bridge configurations and transferring electrons to promote Cr─O bond dissociation, which prominently decreases reaction energy barriers. This work provides a feasible route to boost the stability and robustness of metal single‐atoms that are easily affected by reaction conditions for sustainable catalytic applications.https://doi.org/10.1002/advs.202501393dual‐atom catalystselectrochemical catalysisin situ XAFSsingle‐atom catalystsspring effect |
| spellingShingle | Pei‐Hua Li Yuan‐Fan Yang Zong‐Yin Song Bo Liang Yong‐Huan Zhao Xin Cai Zi‐Hao Liu Jing‐Yi Lin Meng Yang Xiangyu Xiao Jing Zhang Wen‐Qing Liu Xing‐Jiu Huang Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction Advanced Science dual‐atom catalysts electrochemical catalysis in situ XAFS single‐atom catalysts spring effect |
| title | Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction |
| title_full | Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction |
| title_fullStr | Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction |
| title_full_unstemmed | Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction |
| title_short | Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction |
| title_sort | potential driven dynamic spring effect of pd─cu dual atoms empowered stability and activity for electrocatalytic reduction |
| topic | dual‐atom catalysts electrochemical catalysis in situ XAFS single‐atom catalysts spring effect |
| url | https://doi.org/10.1002/advs.202501393 |
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