Anion Constructor for Atomic‐Scale Engineering of Antiperovskite Crystals for Electrochemical Reactions

Among the Pt group metals, Pd has been considered the most efficient for application in electrocatalysts as an alternative to Pt. Despite the comparable electrochemical activities of Pd and Pd‐metal alloys, they are vulnerable to liquid acidic electrolytes, leading to degradation of catalytic activi...

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Bibliographic Details
Published in:Advanced functional materials 2021-04, Vol.31 (16), p.n/a
Main Authors: Lee, Sehyun, Jung, Jae Young, Jang, Injoon, Choi, Daeil, Lee, Myeong Jae, Lee, Dong Wook, Jang, Jue‐Hyuk, Lee, Jeong Hee, Jin, Haneul, Im, Kyungmin, Lee, Eungjun, Kim, Seung‐hoon, Kim, Nam Dong, Lee, Soo‐Hyoung, Kang, Yun Sik, Park, Hee‐Young, Chun, Dongwon, Ham, Hyung Chul, Lee, Kug‐Seung, Ahn, Docheon, Kim, Pil, Yoo, Sung Jong
Format: Article
Language:English
Subjects:
acidic media
atomic‐scale engineering
Catalytic activity
Chemical reactions
Crystal structure
electrocatalysis
Electrocatalysts
electrochemical reactions
Electrolytes
Electronic structure
Free energy
Heat of formation
Materials science
Nanocrystals
Nanoparticles
Nitrides
Nitrogen
Oxygen reduction reactions
Palladium
palladium alloys
Palladium base alloys
Platinum
Stability
Structural analysis
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Summary:Among the Pt group metals, Pd has been considered the most efficient for application in electrocatalysts as an alternative to Pt. Despite the comparable electrochemical activities of Pd and Pd‐metal alloys, they are vulnerable to liquid acidic electrolytes, leading to degradation of catalytic activity. Pd–Ni alloys have been used to enhance catalytic activity because the electronic structure of Pd can be easily changed by adding Ni. In other studies, N atoms have been introduced for more stable M–Ni catalysts by inducing the formation of Ni4N species; however, the structural analysis and the role of nitrogen have not been fully understood yet. Herein, the Pd–Ni alloy nitride with a unique crystal structure shows a promising catalytic activity for oxygen reduction reaction (ORR). The nitride PdNi nanoparticles have a novel monolithic antiperovskite structure of chemical formula (PdxNi1−x)NNi3. The unique antiperovskite crystal (PdxNi1−x)NNi3 possesses superior ORR activity and stability, originating from the downshifted d‐band center of the monolayer Pd/antiperovskite surface and the lower formation energy of the antiperovskite core nanocrystal. Consequently, (PdxNi1−x)NNi3, as a Pt‐free Pd‐based electrocatalyst, overcomes the stability issue of Pd under acidic conditions by achieving 99‐times higher mass activity than commercial Pd/C, as shown by the durability test. Monolithic antiperovskite crystals are synthesized through atomic‐scale engineering. Then nitride PdNi alloy achieves excellent catalytic activity and durability under acidic media, resulting from the synergistic effect of nitride and intermetallic structures. This strategy will pave the way for overcoming the catalytic performance of potential materials.
ISSN:1616-301X
1616-3028
DOI:10.1002/adfm.202009241