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Low-coordinated surface sites make truncated Pd tetrahedrons as robust ORR electrocatalysts outperforming Pt for DMFC devices

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Abstract

Developing highly stable and active non-Pt oxygen reduction reaction (ORR) electrocatalysts for power generation device raises great concerns and remains a challenge. Here, we report novel truncated Pd tetrahedrons (T−Pd−Ths) enclosed by {111} facets with excellent uniformity, which have both low-coordinated surface sites and distinct lattice distortions that would induce “local strain”. In alkaline electrolyte, the T−Pd−Ths/C achieves remarkable ORR specific/mass activity (SA/MA) of 2.46 mA·cm−2/1.69 A·mgPd−1, which is 12.3/16.9 and 10.7/14.1 times higher than commercial Pd/C and Pt/C, respectively. The T−Pd−Ths/C also exhibits high in-situ carbon monoxide (CO) tolerance and 50,000 cycles durability with an activity loss of 7.69% and morphological stability. The rotating ring-disk electrode (RRDE) measurements show that a 4-electron process occurs on T−Pd−Ths/C. Theoretical calculations demonstrate that the low-coordinated surface sites contribute largely to the enhancement of ORR activity. In actual direct methanol fuel cell (DMFC) device, the T−Pd−Ths/C delivers superior open-circuit voltage (OCV) and peak power density (PPD) to commercial Pt/C from 25 to 80 °C, and the maximum PPD can reach up to 163.7 mW·cm−2. This study demonstrates that the T−Pd−Ths/C holds promise as alternatives to Pt for ORR in DMFC device.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21571038), Education Department of Guizhou Province (No. 2021312), Foundation of Guizhou Province (No. 2019-5666), Science Foundation for Aftergraduated Students of Guizhou Province (No. YJSCXJH2020045), State Key Laboratory of Coal Mine Disaster Dynamics and Control (Chongqing University, No. 2011DA105287-ZR202101), State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University, No. 202009), and the Open Fund of the Key Lab of Organic Optoelectronics & Molecular Engineering (Tsinghua University). We gratefully acknowledge Analytical and Testing Center of Chongqing University.

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  1. State-Local Joint Laboratory for Comprehensive Utilization of Biomass, Center for R&D of Fine Chemicals, College of Chemistry and Chemical Engineering, Guizhou University, Guiyang, 550025, China

    Xiaoling Wang, Xiaotong Yang, Fengling Zhao & Qiang Yuan

  2. State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing, 400044, China

    Yongfei Li, Li-Yong Gan & Ke Xin Yao

  3. Key Lab of Organic Optoelectronics & Molecular Engineering, Tsinghua University, Beijing, 100084, China

    Qiang Yuan

  4. Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies & School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China

    Jingwei Li, Daliang Zhang & Ke Xin Yao

  5. College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing, 401331, China

    Li-Yong Gan

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  1. Xiaoling Wang
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Correspondence to Li-Yong Gan, Ke Xin Yao or Qiang Yuan.

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Low-coordinated surface sites make truncated Pd tetrahedrons as robust ORR electrocatalysts outperforming Pt for DMFC devices

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Wang, X., Li, J., Yang, X. et al. Low-coordinated surface sites make truncated Pd tetrahedrons as robust ORR electrocatalysts outperforming Pt for DMFC devices. Nano Res. 15, 7951–7958 (2022). https://doi.org/10.1007/s12274-022-4492-2

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