Volume 137, Issue 30 e202504924
Forschungsartikel

Interface Engineering of Branched PdCoPx Nanostructures for High-Performance Lithium–Oxygen Batteries

Zhiyuan Xu

Zhiyuan Xu

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 China

These authors contributed equally to this work.

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Yu Zhang

Yu Zhang

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 China

These authors contributed equally to this work.

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Hong Yu

Hong Yu

College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060 China

These authors contributed equally to this work.

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Zewen Zhuang

Zewen Zhuang

College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108 China

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Xingdong Wang

Xingdong Wang

Research Institute of Petroleum Processing, SINOPEC, Beijing, 100083 China

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Jiaqi Zhang

Jiaqi Zhang

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Xin Tan

Xin Tan

College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108 China

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Chang Chen

Chang Chen

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 China

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Dr. Xin Chen

Corresponding Author

Dr. Xin Chen

Beijing Advanced Innovation Center for Materials Genome Engineering, Institute of Solid State Chemistry, University of Science and Technology Beijing, Beijing, 100083 China

E-mail: [email protected]; [email protected]; [email protected]

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Prof. Qiuhua Yuan

Corresponding Author

Prof. Qiuhua Yuan

College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060 China

E-mail: [email protected]; [email protected]; [email protected]

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Prof. Chen Chen

Corresponding Author

Prof. Chen Chen

Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 China

E-mail: [email protected]; [email protected]; [email protected]

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First published: 24 May 2025

Abstract

Developing advanced cathode materials plays a positive role in lowering the charge/discharge overpotentials and improving the cycling performance of lithium–oxygen batteries (LOBs). Here we report a direct synthesis strategy to prepare high-dimensional branched PdCoPx series nanostructures, in which the Pd atoms are well dispersed within cobalt phosphide, leading to rich Pd─Co─P interfaces and evoking a prominent ligand effect between the elements. The Pd1Co2Px exhibits an excellent and stable activity for oxygen reduction reaction (ORR) in alkaline media, with a mass activity of 1.46 A mgPd−1, far exceeding that of commercial Pd/C (0.12 A mgPd−1) and Pt/C (0.17 A mgPt−1). Using Pd1Co2Px as the cathode, the resulting LOB shows an ultralow discharge/charge overpotential of 0.40 V and could run stably for over 240 cycles, which is a significant improvement compared with the counterparts using CoPx and Pd/C cathodes. Experimental and density functional theory (DFT) calculation results indicate that the dispersed Pd atoms could significantly enhance the ORR kinetics, and the Pd─Co─P interfaces could direct the two-dimensional growth of Li2O2, thereby facilitating the formation of more easily decomposable film-like Li2O2 products. This feature successfully elevates both the charge and discharge performances, as well as the stability of the LOB.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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