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Synthesis of vanadium-tungsten complex oxides for deNOx catalysts

Research Project

Project/Area Number 20K15092
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionKumamoto University

Principal Investigator

Inomata Yusuke  熊本大学, 大学院先端科学研究部(工), 助教 (40824024)

Project Period (FY) 2020-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2021: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2020: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Keywords脱硝 / NOx / 酸化バナジウム / 酸化タングステン / 環境触媒 / 不均一触媒 / NH3-SCR / ブロンズ化合物 / 窒素酸化物 / 金属酸化物
Outline of Research at the Start

本研究では、窒素酸化物の除去法の一つであるアンモニアを還元剤とした選択的触媒還元 (NH3-SCR) について、低温 (100-150oC) で活性を示す触媒の開発およびその反応メカニズムの解析を目的とする。現在市販化されている脱硝触媒は300oC以上と高い反応温度が必要であり、不活性要因である煤塵および二酸化硫黄 (SO2) を含んだ排ガス上流へ触媒の設置を余儀なくされている。このような背景から本研究では、集じん・脱硫後の排ガス下流への触媒の設置を目指した、100-150oCの低温域で活性を示すタングステン-バナジウム複合酸化物触媒の開発および反応機構の解析をおこなう。

Outline of Final Research Achievements

NH3-SCR (selective catalytic reduction) is important process for conversion of harmful NOx to harmless N2 and H2O. However, the negative effect of water is critical for low-temperature NH3-SCR. In this work, we synthesized bulk W-substituted vanadium oxide catalysts for NH3-SCR at a low temperature and in the presence of water. Vanadium sites were atomically substituted by tungsten for 3.5 mol% W-substituted vanadium oxide. The 3.5mol% W-substituted vanadium oxide showed >99% (dry) and ~93% (wet, 5-20 vol% water) NO conversion at 150oC (250 ppm NO, 250 ppm NH3, 4% O2). Lewis acid sites of W-substituted vanadium oxide were converted to Bronsted acid sites under a wet condition while the distribution of Bronsted and Lewis acid sites did not change without tungsten. The high redox ability and reactivity of Bronsted acid sites were observed for bulk W-substituted vanadium oxide at a low temperature in the presence of water, and thus the catalytic cycle was less affected by water vapor.

Academic Significance and Societal Importance of the Research Achievements

従来の脱硝触媒はその動作に300℃以上の高温が必要であった。本研究では100-150℃程度の低温でも十分なNO転化率を得られる触媒材料を実現した。これにより、従来脱硝触媒材料劣化の点で課題のあった脱硝プロセスで、触媒材料の高寿命化から触媒交換コストの抑制が期待される。学術面では、低温脱硝に求められる触媒材料の性質を反応機構解析から明らかにしたことで、脱硝触媒材料の開発の指針を明確化できた。

Report

(3 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Research-status Report
  • Research Products

    (11 results)

All 2021 2020 Other

All Journal Article (5 results) (of which Peer Reviewed: 5 results,  Open Access: 1 results) Presentation (3 results) Remarks (2 results) Patent(Industrial Property Rights) (1 results) (of which Overseas: 1 results)

  • [Journal Article] Synthesis of bulk vanadium oxide with a large surface area using organic acids and its low-temperature NH3-SCR activity2021

    • Author(s)
      Inomata Yusuke、Hata Shinichi、Kiyonaga Eiji、Morita Keiichiro、Yoshida Kazuhiro、Haruta Masatake、Murayama Toru
    • Journal Title

      Catalysis Today

      Volume: 376 Pages: 188-196

    • DOI

      10.1016/j.cattod.2020.06.041

    • Related Report
      2021 Annual Research Report 2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Synthesis of Zeolitic Mo-Doped Vanadotungstates and Their Catalytic Activity for Low-Temperature NH3-SCR2021

    • Author(s)
      Tao Meilin、Ishikawa Satoshi、Murayama Toru、Inomata Yusuke、Kamiyama Akiho、Ueda Wataru
    • Journal Title

      Inorganic Chemistry

      Volume: 60 Issue: 7 Pages: 5081-5086

    • DOI

      10.1021/acs.inorgchem.1c00107

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Analogous Mechanistic Features of NH3-SCR over Vanadium Oxide and Copper Zeolite Catalysts2021

    • Author(s)
      Kubota Hiroe、Toyao Takashi、Maeno Zen、Inomata Yusuke、Murayama Toru、Nakazawa Naoto、Inagaki Satoshi、Kubota Yoshihiro、Shimizu Ken-ichi
    • Journal Title

      ACS Catalysis

      Volume: 11 Issue: 17 Pages: 11180-11192

    • DOI

      10.1021/acscatal.1c02860

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of Zeolitic Ti, Zr-Substituted Vanadotungstates and Investigation of Their Catalytic Activities for Low Temperature NH3-SCR2021

    • Author(s)
      Tao Meilin、Ishikawa Satoshi、Zhang Zhenxin、Murayama Toru、Inomata Yusuke、Kamiyama Akiho、Nakaima Ichika、Jing Yuan、Mine Shinya、Shimoda Kosuke、Toyao Takashi、Shimizu Ken-ichi、Ueda Wataru
    • Journal Title

      ACS Catalysis

      Volume: 11 Issue: 22 Pages: 14016-14025

    • DOI

      10.1021/acscatal.1c04086

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Bulk tungsten-substituted vanadium oxide for low-temperature NOx removal in the presence of water2021

    • Author(s)
      Inomata Yusuke、Kubota Hiroe、Hata Shinichi、Kiyonaga Eiji、Morita Keiichiro、Yoshida Kazuhiro、Sakaguchi Norihito、Toyao Takashi、Shimizu Ken-ichi、Ishikawa Satoshi、Ueda Wataru、Haruta Masatake、Murayama Toru
    • Journal Title

      Nature Communications

      Volume: 12 Issue: 1 Pages: 557-557

    • DOI

      10.1038/s41467-020-20867-w

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] W置換V2O5触媒による低温・水蒸気雰囲気下でのNH3-SCRと反応機構解析2021

    • Author(s)
      猪股 雄介・清永英嗣・盛田啓一郎・吉田和広・窪田 博愛・鳥屋尾 隆・清水 研一・春田 正毅・村山 徹
    • Organizer
      第127回触媒討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] 水分共存下にて高い低温脱硝作用を示すW添加V2O5触媒2020

    • Author(s)
      猪股 雄介・清永英嗣・盛田啓一郎・吉田和広・窪田 博愛・鳥屋尾 隆・清水 研一・春田 正毅・村山 徹
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Research-status Report
  • [Presentation] 水蒸気存在下での低温脱硝を目指した タングステン添加酸化バナジウム触媒2020

    • Author(s)
      猪股 雄介・清永英嗣・盛田啓一郎・吉田和広・窪田 博愛・鳥屋尾 隆・清水 研一・春田 正毅・村山 徹
    • Organizer
      第50回石油・石油化学討論会
    • Related Report
      2020 Research-status Report
  • [Remarks] EurekAlert!

    • URL

      https://www.eurekalert.org/pub_releases/2021-01/tmu-tvo012021.php

    • Related Report
      2020 Research-status Report
  • [Remarks] 【研究発表】次世代NOx処理システムを開発 ~大気汚染問題に新たな道筋~

    • URL

      https://www.tmu.ac.jp/news/topics/30650.html

    • Related Report
      2020 Research-status Report
  • [Patent(Industrial Property Rights)] Combustion system2021

    • Inventor(s)
      Eiji Kiyonaga et al.
    • Industrial Property Rights Holder
      Eiji Kiyonaga et al.
    • Industrial Property Rights Type
      特許
    • Filing Date
      2021
    • Acquisition Date
      2022
    • Related Report
      2021 Annual Research Report
    • Overseas

URL: 

Published: 2020-04-28   Modified: 2023-01-30  

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