Simultaneous achievement of toxic N-containing compounds removal and syngas recovery via catalytic reforming of product gas from gasfication of N-containing plastic wastes

• Project/Area Number: 17K20057
• Research Category: Grant-in-Aid for Challenging Research (Exploratory)
• Allocation Type: Multi-year Fund
• Research Field: Environmental conservation measure and related fields
• Research Institution: Tohoku University
• Principal Investigator: Kumagai Shogo 東北大学, 環境科学研究科, 助教 (40757598)
• Project Period (FY): 2017-06-30 – 2020-03-31
• Project Status: Completed (Fiscal Year 2019)
• Budget Amount: ¥6,370,000 (Direct Cost: ¥4,900,000、Indirect Cost: ¥1,470,000); Fiscal Year 2019: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000); Fiscal Year 2018: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000); Fiscal Year 2017: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: ポリウレタン / ポリイミド / 熱分解 / ガス化 / シアン化水素分解 / リサイクル / シアン化水素 / ガスクロマトグラフィー / 窒素含有プラスチック / 合成ガス / 有害窒素化合物 / 無害化

Outline of Final Research Achievements

This work conducted pyrolysis of N-containing plastics such as polyurethane and the subsequent catalytic steam reforming of the pyrolyzates including toxic HCN using Ni/Mg/Al catalysts to achieve simultaneous syngas (H2+CO) recovery and toxic HCN decomposition. This approach significantly improved gas production and reduced HCN, from 52 mL/g-sample with 2.8 vol% HCN at pyrolysis condition to 1497 mL/g-sample with 0.5 vol% HCN.

Academic Significance and Societal Importance of the Research Achievements

従来窒素含有プラスチックは熱分解すると有害なシアン化水素を生成するため、熱分解法には不向きのプラスチックと考えられていた。本研究は、ポリウレタンやポリイミドを中心に熱分解反応挙動を詳細に調査し、さらに窒素含有廃プラスチックを合成ガスに転換すると同時にシアン化水素等の有害窒素化合物を同時に無害化することに成功した。窒素含有プラスチックの熱分解機構やHCNの分解反応の理解を深める上で学術的意義のある成果である。さらに、窒素含有廃プラスチックのリサイクルの新しい可能性を見出すことができたため、この社会的意義は極めて大きいと考えている。

Research Products

• [Journal Article] Temperature-dependent pyrolysis behavior of polyurethane elastomers with different hard- and soft-segment compositions (2020)
  • Author(s): Yuya Nishiyama, Shogo Kumagai, Suguru Motokucho, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Hisayuki Nakatani, Toshiaki Yoshioka
  • Journal Title: Journal of Analytical and Applied Pyrolysis Volume: 145 Pages: 104754-104754
  • DOI: 10.1016/j.jaap.2019.104754
  • Peer Reviewed
• [Journal Article] Hydrogen and steam injected tandem μ-reactor GC/FID system: phenol recovery from bisphenol A and alkylphenols using Ni/Y zeolite (2019)
  • Author(s): Shogo Kumagai, Masaki Asakawa, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Chuichi Watanabe, Norio Teramae, Toshiaki Yoshioka
  • Journal Title: Reaction Chemistry & Engineering Volume: 4 Issue: 12 Pages: 2099-2107
  • DOI: 10.1039/c9re00299e
  • Peer Reviewed
• [Journal Article] Simultaneous recovery of H2-rich syngas and removal of HCN during pyrolytic recycling of polyurethane by Ni/Mg/Al catalysts (2019)
  • Author(s): Shogo Kumagai, Ryosuke Yabuki, Tomohito Kameda, Yuko Saito, Toshiaki Yoshioka
  • Journal Title: Chemical Engineering Journal Volume: 361 Pages: 408-415
  • DOI: 10.1016/j.cej.2018.12.099
  • Peer Reviewed
• [Journal Article] Selective phenol recovery via simultaneous hydrogenation/dealkylation of isopropyl- and isopropenyl-phenols employing an H2 generator combined with tandem micro-reactor GC/MS (2018)
  • Author(s): Kumagai Shogo、Asakawa Masaki、Kameda Tomohito、Saito Yuko、Watanabe Atsushi、Watanabe Chuichi、Teramae Norio、Yoshioka Toshiaki
  • Journal Title: Scientific Reports Volume: 8 Issue: 1 Pages: 13994-13994
  • DOI: 10.1038/s41598-018-32269-6
  • Peer Reviewed / Open Access
• [Journal Article] Aromatic hydrocarbon selectivity as a function of CaO basicity and aging during CaO-catalyzed PET pyrolysis using tandem micro-reactor-GC/MS (2018)
  • Author(s): Shogo Kumagai, Ryota Yamasaki, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Chuichi Watanabe, Norio Teramae, Toshiaki Yoshioka
  • Journal Title: Chemical Engineering Journal Volume: 332 Pages: 169-173
  • DOI: 10.1016/j.cej.2017.09.077
  • Peer Reviewed
• [Journal Article] Effects of hard- and soft-segment composition on pyrolysis characteristics of MDI, BD, and PTMG-based polyurethane elastomers (2017)
  • Author(s): Shogo Kumagai, Suguru Motokucho, Ryosuke Yabuki, Airi Anzai, Tomohito Kameda, Atsushi Watanabe, Hisayuki Nakatani, Toshiaki Yoshioka
  • Journal Title: Journal of Analytical and Applied Pyrolysis Volume: 126 Pages: 337-345
  • DOI: 10.1016/j.jaap.2017.05.012
  • Peer Reviewed
• [Journal Article] Tandem μ-reactor-GC/MS for online monitoring of aromatic hydrocarbon production via CaO-catalysed PET pyrolysis (2017)
  • Author(s): Shogo Kumagai, Ryota Yamasaki, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Chuichi Watanabe, Norio Teramae, Toshiaki Yoshioka
  • Journal Title: Reaction Chemistry & Engineering Volume: 2 Issue: 5 Pages: 776-784
  • DOI: 10.1039/c7re00097a
  • Peer Reviewed
• [Presentation] タンデムマイクロリアクター-GC/MSを用いた熱分解生成物の気相誘導体化 (2019)
  • Author(s): 西山雄也, 熊谷将吾, 亀田知人, 齋藤優子, 渡辺壱, 本九町卓, 中谷久之, 吉岡敏明
  • Organizer: 第24回高分子分析討論会
• [Presentation] プラスチックのケミカルリサイクルへの熱分解法の応用 (2019)
  • Author(s): 熊谷将吾, 亀田知人, 齋藤優子, 吉岡敏明
  • Organizer: 第68回高分子討論会
  • Invited
• [Presentation] プラスチックを取り巻く状況およびリサイクル技術の研究開発 (2019)
  • Author(s): 熊谷将吾
  • Organizer: 東北大学-DOWA技術者交流会
  • Invited
• [Presentation] Simultaneous Achievement of Syngas Recovery and Toxic HCN Removal through Catalytic Gasification of Polyurethanes (2019)
  • Author(s): Shogo Kumagai, Ryosuke Yabuki, Tomohito Kameda, Yuko Saito, Toshiaki Yoshioka
  • Organizer: 1st International Symposium on Electronic Waste and End-of-Life Vehicles
  • Int'l Joint Research
• [Presentation] Pyrolysis for Feedstock recycling of plastic wastes (2019)
  • Author(s): Shogo Kumagai
  • Organizer: 1st International Symposium on Analytical and Applied Pyrolysis in the Asian Region
  • Int'l Joint Research / Invited
• [Presentation] H2-rich syngas recovery and HCN removal via catalytic reforming of product gas from thermal degradation of polyurethanes over Ni/Mg/Al catalyst (2019)
  • Author(s): Shogo Kumagai, Ryosuke Yabuki, Tomohito Kameda, Yuko Saito, Toshiaki Yoshioka
  • Organizer: 5th 3R International Scientific Conference on Material Cycles and Waste Management
  • Int'l Joint Research
• [Presentation] MDI、BD、PTMG組成の異なるポリウレタンエラストマーの熱分解 (2019)
  • Author(s): 西山雄也、熊谷将吾、亀田知人、齋藤優子、渡辺壱、本九町卓、中谷久之、吉岡敏明
  • Organizer: 第11回廃棄物資源循環学会東北支部第6回日本水環境学会東北支部合同研究発表会
• [Presentation] 環境科学に立脚した高分子の熱分解反応解析 (2018)
  • Author(s): 熊谷将吾
  • Organizer: 日本分析化学会第67年会
  • Invited
• [Presentation] ポリウレタンエラストマーの熱分解挙動に及ぼすハードセグメント比率の影響 (2018)
  • Author(s): 西山雄也、熊谷将吾、亀田知人、齋藤優子、渡辺壱、本九町卓、中谷久之、吉岡敏明
  • Organizer: 第７回高分子学会グリーンケミストリー研究会シンポジウム、第２１回プラスチックリサイクル化学研究会討論会 合同発表会
• [Presentation] Tandem μ-reactor-GC/MSによる高分子の熱分解ー触媒反応の解析 (2018)
  • Author(s): 熊谷将吾、山崎僚太、浅川将輝、亀田知人、齋藤優子、渡辺壱、吉岡敏明
  • Organizer: 第７回高分子学会グリーンケミストリー研究会シンポジウム、第２１回プラスチックリサイクル化学研究会討論会 合同発表会
• [Presentation] Online Products Monitoring during Two-Step PET Pyrolysis-Calcium Oxide Reaction Using Tandem μ-Reactor-GC/MS (2018)
  • Author(s): Shogo Kumagai, Ryota Yamasaki, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Norio Teramae, Toshiaki Yoshioka
  • Organizer: 22nd International Symposium on Analytical and Applied Pyrolysis
  • Int'l Joint Research
• [Presentation] Tandem μ-reactor-GC/MS for screening of zeolite catalysts for dealkylation of alkylphenols (2018)
  • Author(s): Masaki Asakawa, Shogo Kumagai, Tomohito Kameda, Yuko Saito, Atsushi Watanabe, Norio Teramae, Toshiaki Yoshioka
  • Organizer: 22nd International Symposium on Analytical and Applied Pyrolysis
  • Int'l Joint Research
• [Presentation] 高分子の熱分解研究の方法論および応用分野 (2018)
  • Author(s): 熊谷将吾
  • Organizer: 第10回 製鉄・資源に関するWorkshop（還元研究会）
  • Invited
• [Presentation] Tandem μ-reactor-GC/MS for evaluation of solid acid- and base-catalysts performance (2018)
  • Author(s): Shogo Kumagai
  • Organizer: Frontier Seminar
  • Int'l Joint Research / Invited
• [Presentation] ゼオライト触媒を用いたアルキルフェノールのフェノール転換反応挙動の評価におけるタンデム μ-リアクターの応用 (2018)
  • Author(s): 浅川将輝、熊谷将吾、亀田知人、齋藤優子、渡辺壱、寺前紀夫、吉岡敏明
  • Organizer: 日本化学会第98春季年会
• [Presentation] Syngas reovery during steam gasification of polyurethane using Ni/Mg/Al catalysts (2017)
  • Author(s): Ryosuke Yabuki, Shogo Kumagai, Tomohito Kameda, Toshiaki Yoshioka
  • Organizer: 21th Korea-Japan Joint International Session
  • Int'l Joint Research
• [Presentation] Benzene recovery from poly(ethylene terephthalate) using CaO with different activities (2017)
  • Author(s): Ryota Yamasaki, Shogo Kumagai, Tomohito Kameda, Toshiaki Yoshioka
  • Organizer: 21th Korea-Japan Joint International Session
  • Int'l Joint Research
• [Presentation] H2-rich syngas recovery and toxic HCN removal from N-containing plastics using Ni catalysts (2017)
  • Author(s): Shogo Kumagai, Tomoyuki Hosaka, Tomohito Kameda, Toshiaki Yoshioka
  • Organizer: 9th International Symposium on Feedstock Recycling of Polymeric Materials
  • Int'l Joint Research
• [Presentation] タンデムμ-リアクター-GC/MSによるアルキルフェノールの脱アルキル化に向けたゼオライト触媒のスクリーニング (2017)
  • Author(s): 浅川将輝, 熊谷将吾, 亀田知人, 渡辺壱, 寺前紀夫, 吉岡敏明
  • Organizer: 日本分析化学会第66年会
• [Presentation] タンデムμ-リアクター-GC/MSによるポリエチレンテレフタレート油化生成物のオンライン分析 (2017)
  • Author(s): 熊谷将吾, 山崎僚太, 亀田知人, 渡辺壱, 寺前紀夫, 吉岡敏明
  • Organizer: 日本分析化学会第66年会
• [Presentation] Selective conversion of isopropyl phenol and isopropenyl phenol into phenol using zeolite catalysis (2017)
  • Author(s): 浅川将輝, 熊谷将吾, 亀田知人, 渡辺壱, 寺前紀夫, 吉岡敏明
  • Organizer: 平成29年度化学系学協会東北大会
• [Presentation] タンデムμ-リアクター-GC/MSによるPET熱分解/CaO改質二段プロセスの反応機構解析 (2017)
  • Author(s): 熊谷将吾, 山崎僚太, 亀田知人, 渡辺壱, 寺前紀夫, 吉岡敏明
  • Organizer: 第22回高分子分析討論会
• [Presentation] Pyrolysis I : Methodology for conducting analytical pyrolysis of polymers (2017)
  • Author(s): Shogo Kumagai
  • Organizer: Special lectures for Department of Chemical Engineering students and staffs
  • Int'l Joint Research / Invited
• [Book] 生分解、バイオマスプラスチックの開発と応用（第８章第２節担当） (2020)
  • Author(s): 熊谷将吾, 亀田知人, 齋藤優子, 吉岡敏明
  • Total Pages: 560
  • Publisher: 技術情報協会
  • ISBN: 9784861047824