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2020 年度 実施状況報告書

Ambient-Pressure synchrotron X-ray study to reveal atomic-scale mechanism of CO oxidation and three-way catalytic reaction of Ru based solid-solution nanoparticles

研究課題

研究課題/領域番号 20K15083
研究機関国立研究開発法人物質・材料研究機構

研究代表者

徐 玉均  国立研究開発法人物質・材料研究機構, 技術開発・共用部門, NIMSポスドク研究員 (30814206)

研究期間 (年度) 2020-04-01 – 2022-03-31
キーワードH absorption / CO oxidation / three-way catalysts / EXAFS / AP-XPS
研究実績の概要

Rh is a material that does not absorb hydrogen atoms. However, when the particle size of the Rh materials becomes small, hydrogen adsorption on the surface area of the Rh nanoparticles is possible due to surface disordering of the Rh nanoparticles. Besides, as the size of Rh nanoparticles increases, hydrogen adsorption on the Rh nanoparticles occurs less than that of the small size, measured by dispersive XAFS. (RSC Adv.)
The change in the atomic arrangement at the interface on the bimetallic alloy (AgRh and PdPt) nanoparticles were investigated using the in-situ EXAFS measurement under hydrogen conditions.The research results were published in the J. Alloys Compd. and ACS Appl. Mater. Interface as research articles.
AgRh nanoparticles: A substantial fraction of the sample is an alloy phase formed by mixing of nano/sub-nanosized domains of Rh and Ag NPs. Mixing at the atomic level mainly occurs in the interfacial region. Consequently, the interfacial region has an important influence over the microstructure and provides active sites for hydrogen absorption.
PdPt nanoparticles: The Pd K-edge extended X-ray absorption fine structure data indicate that in CS and SS NPs a substantial fraction of the signal derives from Pd-Pd atomic pairs, indicating that Pd clusters remain present even after hydrogen absorptin and desorption process. Hydrogen absorption and desorption process on the PdPt nanoparticles causes a atomic rearrangement of the interfacial structure,which becomes homogeneously distributed.

現在までの達成度 (区分)
現在までの達成度 (区分)

1: 当初の計画以上に進展している

理由

In 2020, we have been studied the oxidation and reduction reaction process through dispersive XAFS and in-situ XAFS experiments at Pd K edge, Ru K edge, and Ce L3 edge at 300 and 400 C to investigate the three-way catalysts (lean-rich-stoichiometry conditions) mechanism of PdRu nanoparticles-CeO2ZrO2 (CZ). In addition, we were conducted the in-situ XAFS experiment under CO and CO oxidation conditions at 100, 150, and 200 C to investigate the reaction site of the PdRu nanoparticles-CZ. I am preparing the research articles on the three-way catalytic reactoin of the PdRu nanoparticles-CZ.

To understand the atomic behavior of the PdRu nanoparticles under CO oxidation, ambient pressure XPS (AP-XPS) was performed at Pohang Accelerator Laboratory in Korea. We found the surface segregation of specific atoms during CO, O2, and CO oxidation conditions. Surface segregation of the metal atoms in the alloy nanoparticles is important evidence to know the adsorption sites of metals under the CO oxidation reaction.

今後の研究の推進方策

Three-way catalsts: The evaporation of Ru in PdRu nanoparticles is the reason why the three-way catalytic performance of PdRu nanoparticles decreases at high temperatures. To prevent evaporation of Ru at high operation temperature, we synthesized PdRuIr nanoparticles, as a ternary alloy. Kusada et al., reported that the PdRuIr nanoparticles was stable at the high temperature. (Adv. Mater. 33, 2005206 (2021))Therefore, the dispersive XAFS and in-situ XAFS experiments will be conducted to find out the mechanism by which the performance of the ternary PdRuIr nanoparticles increases.

CO oxidation: The AP-XPS experiment will be conducted to investigate the surface atomic behaviors of hcp and fcc structure PtRu nanoparticles under CO oxidation. In addition, we are planning to observe the CO oxidation effect caused by the crystal structure of hcp and fcc structure. Because I cannot go to Pohang Accelerator Laboratory due to COVID 19, the AP-XPS experiment will be performed by a research collaborator.

次年度使用額が生じた理由

From April 2021, I moved the research Institute from NIMS to JASRI.
Therefore, I am planning to purchase the equipment for HAXPES beamline and XAFS experiment, including the in-situ equipment. In addition, I am planning to use the other beamtime fee (XAFS beamline) and publication fee of research articles, which related to the research of the metal nanoparticles. Due to COVID 19, it is impossible to participate in experiments and conferences in foreign countries, so I will use the remaining money to develop the in-situ synchrotron X-ray technique equipments.
HAXPES: Sample holder for in-situ experiment, pelletizer
XAFS: Beamtime fee, stainless holder, gas

  • 研究成果

    (11件)

すべて 2021 2020 その他

すべて 雑誌論文 (10件) (うち国際共著 10件、 査読あり 10件、 オープンアクセス 5件) 備考 (1件)

  • [雑誌論文] Investigation of microstructure and hydrogen absorption properties of bulk immiscible AgRh alloy nanoparticles2021

    • 著者名/発表者名
      Tayal Akhil、Seo Okkyun、Kim Jaemyung、Kusada Kohei、Kobayashi Hirokazu、Kitagawa Hiroshi、Sakata Osami
    • 雑誌名

      Journal of Alloys and Compounds

      巻: 869 ページ: 159268~159268

    • DOI

      10.1016/j.jallcom.2021.159268

    • 査読あり / 国際共著
  • [雑誌論文] Mechanism of Hydrogen Storage and Structural Transformation in Bimetallic Pd?Pt Nanoparticles2021

    • 著者名/発表者名
      Tayal Akhil、Seo Okkyun、Kim Jaemyung、Kobayashi Hirokazu、Yamamoto Tomokazu、Matsumura Syo、Kitagawa Hiroshi、Sakata Osami
    • 雑誌名

      ACS Applied Materials & Interfaces

      巻: 13 ページ: 23502~23512

    • DOI

      10.1021/acsami.0c22432

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Efficient overall water splitting in acid with anisotropic metal nanosheets2021

    • 著者名/発表者名
      Wu Dongshuang、Kusada Kohei、Yoshioka Satoru、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Chen Yanna、Seo Okkyun、Kim Jaemyung、Song Chulho、Hiroi Satoshi、Sakata Osami、Ina Toshiaki、Kawaguchi Shogo、Kubota Yoshiki、Kobayashi Hirokazu、Kitagawa Hiroshi
    • 雑誌名

      Nature Communications

      巻: 12 ページ: 1145 ~ 1145

    • DOI

      10.1038/s41467-021-20956-4

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Non-oxidative propane dehydrogenation over alumina-supported Co-V oxide catalysts2021

    • 著者名/発表者名
      Jeon Namgi、Seo Okkyun、Oh Jungmok、Park Jisu、Chung Iljun、Kim Jaemyung、Sakata Osami、Tayal Akhil、Yun Yongju
    • 雑誌名

      Applied Catalysis A: General

      巻: 614 ページ: 118036~118036

    • DOI

      10.1016/j.apcata.2021.118036

    • 査読あり / 国際共著
  • [雑誌論文] Highly Stable and Active Solid‐Solution‐Alloy Three‐Way Catalyst by Utilizing Configurational‐Entropy Effect2021

    • 著者名/発表者名
      Kusada K.、Wu D.、Nanba Y.、Koyama M.、Yamamoto T.、Tran X. Q.、Toriyama T.、Matsumura S.、Ito A.、Sato K.、Nagaoka K.、Seo O.、Song C.、Chen Y.、Palina N.、Kumara L. S. R.、Hiroi S.、Sakata O.、Kawaguchi S.、Kubota Y.、Kitagawa H.
    • 雑誌名

      Advanced Materials

      巻: 33 ページ: 2005206~2005206

    • DOI

      10.1002/adma.202005206

    • 査読あり / 国際共著
  • [雑誌論文] Highly-crystalline 6 inch free-standing GaN observed using X-ray diffraction topography2021

    • 著者名/発表者名
      Kim Jaemyung、Seo Okkyun、Kumara L. S. R.、Nabatame Toshihide、Koide Yasuo、Sakata Osami
    • 雑誌名

      CrystEngComm

      巻: 23 ページ: 1628~1633

    • DOI

      10.1039/d0ce01572e

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Hydrogen absorption and desorption on Rh nanoparticles revealed by in situ dispersive X-ray absorption fine structure spectroscopy2020

    • 著者名/発表者名
      Song Chulho、Seo Okkyun、Matsumura Daiju、Hiroi Satoshi、Cui Yi-Tao、Kim Jaemyung、Chen Yanna、Tayal Akhil、Kusada Kohei、Kobayashi Hirokazu、Kitagawa Hiroshi、Sakata Osami
    • 雑誌名

      RSC Advances

      巻: 10 ページ: 19751~19758

    • DOI

      10.1039/d0ra03322g

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Modifying the crystal structures of Fe2O3-doped NiO epitaxial thin films grown at room temperature by controlling the oxygen partial pressure2020

    • 著者名/発表者名
      Seo Okkyun、Tayal Akhil、Kim Jaemyung、Song Chulho、Katsuya Yoshio、Sakata Osami、Tang Jiayi、Lee Nodo、Kim Yong Tae、Ikeya Yuki、Takano Shiori、Matsuda Akifumi、Yoshimoto Mamoru
    • 雑誌名

      Applied Surface Science

      巻: 533 ページ: 147432~147432

    • DOI

      10.1016/j.apsusc.2020.147432

    • 査読あり / 国際共著
  • [雑誌論文] On the electronic structure and hydrogen evolution reaction activity of platinum group metal-based high-entropy-alloy nanoparticles2020

    • 著者名/発表者名
      Wu Dongshuang、Kusada Kohei、Yamamoto Tomokazu、Toriyama Takaaki、Matsumura Syo、Gueye Ibrahima、Seo Okkyun、Kim Jaemyung、Hiroi Satoshi、Sakata Osami、Kawaguchi Shogo、Kubota Yoshiki、Kitagawa Hiroshi
    • 雑誌名

      Chemical Science

      巻: 11 ページ: 12731~12736

    • DOI

      10.1039/d0sc02351e

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Crystalline to amorphous transformation in solid-solution alloy nanoparticles induced by boron doping2020

    • 著者名/発表者名
      Kobayashi Keigo、Kusada Kohei、Wu Dongshuang、Ogiwara Naoki、Kobayashi Hirokazu、Haruta Mitsutaka、Kurata Hiroki、Hiroi Satoshi、Seo Okkyun、Song Chulho、Chen Yanna、Kim Jaemyung、Tayal Akhil、Sakata Osami、Ohara Koji、Honma Tetsuo、Kitagawa Hiroshi
    • 雑誌名

      Chemical Communications

      巻: 56 ページ: 12941~12944

    • DOI

      10.1039/d0cc05418f

    • 査読あり / 国際共著
  • [備考] google scholar

    • URL

      https://scholar.google.co.kr/citations?user=nlxZevAAAAAJ&hl=ko

URL: 

公開日: 2021-12-27  

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