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

机译：用于电化学反应的Atiperovskite晶体原子尺度工程的阴离子构造函数

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摘要

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.
机译：间的铂族金属，钯一直被认为是最有效的应用在电催化剂作为替代铂。尽管Pd和Pd的金属合金的电化学可比的活动，它们很容易受到液体酸性电解质，导致催化活性的劣化。钯镍合金已被用于增强的催化活性，因为钯的电子结构可通过添加Ni来容易地改变。在其他研究中，N原子已被引入用于更稳定的M-Ni催化剂的通过诱导Ni4N物种的形成;然而，结构分析和氮的作用尚未完全被了解。本文中，Pd-Ni合金的氮化物具有独特的晶体结构示出了用于氧还原反应（ORR）有希望的催化活性。氮化物钯镍纳米颗粒具有化学式（PdxNi1-x）的NNi3的一种新颖的单片antiperovskite结构。独特antiperovskite晶体（PdxNi1-x）的NNi3具有优异ORR活性和稳定性，源自单层的Pd / antiperovskite表面的降档d带中心和antiperovskite核纳米晶体的下部形成能。因此，（PdxNi1-x）的NNi3，作为Pt的自由基于Pd的电催化剂，通过实现比商业的Pd / C 99倍更高的质量活性，如由耐久性试验克服在酸性条件下的Pd的稳定性问题。

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  • 来源
    《Advanced Functional Materials》 |2021年第16期|2009241.1-2009241.9|共9页
  • 作者

    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;

  • 作者单位

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol KIST Funct Composite Mat Res Ctr Wanju Gun 55324 South Korea|Jeonbuk Natl Univ Sch Chem Engn Jeonju 54896 South Korea|Gwangju Inst Sci & Technol GIST Sch Mat Sci & Engn Gwangju 61005 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea|Seoul Natl Univ Sch Chem & Biol Engn Seoul 08826 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea|Korea Univ Green Sch Grad Sch Energy & Environm Seoul 02792 South Korea;

    Korea Inst Sci & Technol KIST Funct Composite Mat Res Ctr Wanju Gun 55324 South Korea;

    Jeonbuk Natl Univ Sch Chem Engn Jeonju 54896 South Korea;

    Hyundai Mobis Fuel Cell Engn Team Uiwang 16082 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea;

    Korea Inst Sci & Technol KIST Adv Anal Ctr Seoul 02792 South Korea;

    Inha Univ Dept Chem Engn Incheon 22212 South Korea;

    Pohang Accelerator Lab Pohang 37673 South Korea;

    Pohang Accelerator Lab Pohang 37673 South Korea;

    Jeonbuk Natl Univ Sch Chem Engn Jeonju 54896 South Korea;

    Korea Inst Sci & Technol Ctr Hydrogen Fuel Cell Res Seoul 02792 South Korea|Kyung Hee Univ KHU KIST Dept Converging Sci & Technol Seoul 02447 South Korea|Univ Sci & Technol UST KIST Sch Div Energy & Environm Technol Seoul 02792 South Korea;

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  • 正文语种 eng
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  • 关键词

    acidic media; atomic-scale engineering; electrocatalysis; electrochemical reactions; palladium alloys;

    机译：酸性介质;原子尺度工程;电殖分析;电化学反应;钯合金;

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