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 () and Yang Yang ()
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Jinfa Chang: University of Central Florida
Guanzhi Wang: University of Central Florida
Maoyu Wang: Oregon State University
Qi Wang: Southern University of Science and Technology
Boyang Li: University of Pittsburgh
Hua Zhou: Argonne National Laboratory
Yuanmin Zhu: Southern University of Science and Technology
Wei Zhang: University of Central Florida
Mahmoud Omer: University of Central Florida
Nina Orlovskaya: University of Central Florida
Qing Ma: Advanced Photon Source
Meng Gu: Southern University of Science and Technology
Zhenxing Feng: Oregon State University
Guofeng Wang: University of Pittsburgh
Yang Yang: University of Central Florida

Nature Energy, 2021, vol. 6, issue 12, 1144-1153

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41560-021-00940-4

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