Improving Pd–N–C fuel cell electrocatalysts through fluorination-driven rearrangements of local coordination environment

Jinfa Chang; Guanzhi Wang; Maoyu Wang; Qi Wang; Boyang Li; Hua Zhou; Yuanmin Zhu; Wei Zhang; Mahmoud Omer; Nina Orlovskaya; Qing Ma; Meng Gu; Zhenxing Feng; Guofeng Wang; Yang Yang

doi:10.1038/s41560-021-00940-4

Improving Pd–N–C fuel cell electrocatalysts through fluorination-driven rearrangements of local coordination environment

Jinfa Chang
, Guanzhi Wang
, Maoyu Wang
, Qi Wang
, Boyang Li
, Hua Zhou
, Yuanmin Zhu
, Wei Zhang
, Mahmoud Omer
, Nina Orlovskaya
, Qing Ma
, Meng Gu^*
, Zhenxing Feng^*
, Guofeng Wang^*
, Yang Yang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

223 Citations (Scopus)

Abstract

The local coordination environment around catalytically active sites plays a vital role in tuning the activity of electrocatalysts made of carbon-supported metal nanoparticles. However, the rational design of electrocatalysts with improved performance by controlling this environment is hampered by synthetic limitations and insufficient mechanistic understanding of how the catalytic phase forms. Here we show that introducing F atoms into Pd/N–C catalysts modifies the environment around the Pd and improves both activity and durability for the ethanol oxidation reaction and the oxygen reduction reaction. Our data suggest that F atom introduction creates a more N-rich Pd surface, which is favourable for catalysis. Durability is enhanced by inhibition of Pd migration and decreased carbon corrosion. A direct ethanol fuel cell that uses the Pd/N–C catalyst with F atoms introduced for both the ethanol oxidation reaction and oxygen reduction reaction achieves a maximum power density of 0.57 W cm⁻² and more than 5,900 hours of operation. Pd/C catalysts containing other heteroatoms (P, S, B) can also be improved through the addition of F atoms. © 2021, The Author(s), under exclusive licence to Springer Nature Limited.

Original language	English
Pages (from-to)	1144-1153
Number of pages	10
Journal	Nature Energy
Volume	6
Issue number	12
Online published	29 Nov 2021
DOIs	https://doi.org/10.1038/s41560-021-00940-4
Publication status	Published - Dec 2021
Externally published	Yes

Funding

This work was supported by a start-up grant from the University of Central Florida. J.C. acknowledges financial support from the Preeminent Postdoctoral Program (P3) at the University of Central Florida. The XPS test was supported by the US National Science Foundation (Division of Electrical, Communications and Cyber Systems, no. 1726636), hosted in the Materials Characterization Facility and Advanced Materials Processing and Analysis Center, Department of Materials Science and Engineering, College of Engineering and Computer Science, University of Central Florida. Z.F. acknowledges support from the US National Science Foundation (National Nanotechnology Coordinated Infrastructure, no. 2025489). Guofeng Wang and B.L. acknowledge support from the US National Science Foundation (Division of Chemical, Bioengineering, Environmental and Transport Systems, no. 1804534). Computational resources were provided by the University of Pittsburgh Center for Research Computing as well as the Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation grant no. ACI-1053575. The use of the Advanced Photon Source at Argonne National Laboratory for XAS measurements at beamlines 5-BM and 12-BM was supported by the US Department of Energy under contract no. DE-AC02-06CH11357. DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) is supported through E. I. duPont de Nemours and Company, Northwestern University and the Dow Chemical Company. M.G. acknowledges support from the Guangdong Innovative and Entrepreneurial Research Team Program (grant no. 2019ZT08C044) and the Peacook Team Program supported by the Science, Technology and Innovation Commission of Shenzhen Municipality (KQTD20190929173815000).

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This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

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title = "Improving Pd–N–C fuel cell electrocatalysts through fluorination-driven rearrangements of local coordination environment",

abstract = "The local coordination environment around catalytically active sites plays a vital role in tuning the activity of electrocatalysts made of carbon-supported metal nanoparticles. However, the rational design of electrocatalysts with improved performance by controlling this environment is hampered by synthetic limitations and insufficient mechanistic understanding of how the catalytic phase forms. Here we show that introducing F atoms into Pd/N–C catalysts modifies the environment around the Pd and improves both activity and durability for the ethanol oxidation reaction and the oxygen reduction reaction. Our data suggest that F atom introduction creates a more N-rich Pd surface, which is favourable for catalysis. Durability is enhanced by inhibition of Pd migration and decreased carbon corrosion. A direct ethanol fuel cell that uses the Pd/N–C catalyst with F atoms introduced for both the ethanol oxidation reaction and oxygen reduction reaction achieves a maximum power density of 0.57 W cm−2 and more than 5,900 hours of operation. Pd/C catalysts containing other heteroatoms (P, S, B) can also be improved through the addition of F atoms. {\textcopyright} 2021, The Author(s), under exclusive licence to Springer Nature Limited.",

author = "Jinfa Chang and Guanzhi Wang and Maoyu Wang and Qi Wang and Boyang Li and Hua Zhou and Yuanmin Zhu and Wei Zhang and Mahmoud Omer and Nina Orlovskaya and Qing Ma and Meng Gu and Zhenxing Feng and Guofeng Wang and Yang Yang",

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AU - Chang, Jinfa

AU - Wang, Guanzhi

AU - Wang, Maoyu

AU - Wang, Qi

AU - Li, Boyang

AU - Zhou, Hua

AU - Zhu, Yuanmin

AU - Zhang, Wei

AU - Omer, Mahmoud

AU - Orlovskaya, Nina

AU - Ma, Qing

AU - Gu, Meng

AU - Feng, Zhenxing

AU - Wang, Guofeng

AU - Yang, Yang

PY - 2021/12

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N2 - The local coordination environment around catalytically active sites plays a vital role in tuning the activity of electrocatalysts made of carbon-supported metal nanoparticles. However, the rational design of electrocatalysts with improved performance by controlling this environment is hampered by synthetic limitations and insufficient mechanistic understanding of how the catalytic phase forms. Here we show that introducing F atoms into Pd/N–C catalysts modifies the environment around the Pd and improves both activity and durability for the ethanol oxidation reaction and the oxygen reduction reaction. Our data suggest that F atom introduction creates a more N-rich Pd surface, which is favourable for catalysis. Durability is enhanced by inhibition of Pd migration and decreased carbon corrosion. A direct ethanol fuel cell that uses the Pd/N–C catalyst with F atoms introduced for both the ethanol oxidation reaction and oxygen reduction reaction achieves a maximum power density of 0.57 W cm−2 and more than 5,900 hours of operation. Pd/C catalysts containing other heteroatoms (P, S, B) can also be improved through the addition of F atoms. © 2021, The Author(s), under exclusive licence to Springer Nature Limited.

AB - The local coordination environment around catalytically active sites plays a vital role in tuning the activity of electrocatalysts made of carbon-supported metal nanoparticles. However, the rational design of electrocatalysts with improved performance by controlling this environment is hampered by synthetic limitations and insufficient mechanistic understanding of how the catalytic phase forms. Here we show that introducing F atoms into Pd/N–C catalysts modifies the environment around the Pd and improves both activity and durability for the ethanol oxidation reaction and the oxygen reduction reaction. Our data suggest that F atom introduction creates a more N-rich Pd surface, which is favourable for catalysis. Durability is enhanced by inhibition of Pd migration and decreased carbon corrosion. A direct ethanol fuel cell that uses the Pd/N–C catalyst with F atoms introduced for both the ethanol oxidation reaction and oxygen reduction reaction achieves a maximum power density of 0.57 W cm−2 and more than 5,900 hours of operation. Pd/C catalysts containing other heteroatoms (P, S, B) can also be improved through the addition of F atoms. © 2021, The Author(s), under exclusive licence to Springer Nature Limited.

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Improving Pd–N–C fuel cell electrocatalysts through fluorination-driven rearrangements of local coordination environment

Abstract

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