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Nano Research 2022, 15(9): 7951-7958 https://doi.org/10.1007/s12274-022-4492-2
Research Article | Issue | Published: 23 June 2022

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

Show Author's Information Xiaoling Wang1,  Jingwei Li4,  Xiaotong Yang1,  Fengling Zhao1,  Yongfei Li2,  Daliang Zhang4,  Li-Yong Gan2,5( ),  Ke Xin Yao2,4( ),  Qiang Yuan1,3( )
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
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China
Key Lab of Organic Optoelectronics & Molecular Engineering, Tsinghua University, Beijing 100084, China
Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies & School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China
Keywords:
oxygen reduction reaction, direct methanol fuel cells, Pd tetrahedrons, low-coordinated sites, lattice distortion
Topics:
Electrocatalysts
Cite this article:
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 Research, 2022, 15(9): 7951-7958. https://doi.org/10.1007/s12274-022-4492-2
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Abstract Full text Electronic supplementary material About this article

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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Electronic supplementary material
About this article

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

Show Author's information Xiaoling Wang1, Jingwei Li4, Xiaotong Yang1, Fengling Zhao1, Yongfei Li2, Daliang Zhang4, Li-Yong Gan2,5( ), Ke Xin Yao2,4( ), Qiang Yuan1,3( )
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
State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China
Key Lab of Organic Optoelectronics & Molecular Engineering, Tsinghua University, Beijing 100084, China
Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies & School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
College of Physics and Center of Quantum Materials and Devices, Chongqing University, Chongqing 401331, China

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.

Keywords: oxygen reduction reaction, direct methanol fuel cells, Pd tetrahedrons, low-coordinated sites, lattice distortion

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Acknowledgements

Publication history

Received: 29 March 2022
Revised: 24 April 2022
Accepted: 01 May 2022
Published: 23 June 2022
Issue date: September 2022

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© Tsinghua University Press 2022

Acknowledgements

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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