Anion constructor for atomic-scale engineering of antiperovskite crystals for electrochemical reactions
- Anion constructor for atomic-scale engineering of antiperovskite crystals for electrochemical reactions
- 천동원; 유성종; 김남동; 박희영; 이세현; 이명재; 장인준; 장주혁; 이동욱; 김승훈; 진하늘; 최대일; 이정희; 임경민; 이응준; 정재영; 이수형; 강윤식; 함형철; 이국승; 안도천; 김필
- acidic media; atomic-scale engineering; electrocatalysis; electrochemical reactions; palladium alloys
- Issue Date
- Advanced functional materials
- VOL 31, NO 16, 2009241
- 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.
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