Development of Advanced Technique to Measure the Solid Acidity and Derived Study on the Acid Site Generation Mechanism

• Project/Area Number: 18206082
• Research Category: Grant-in-Aid for Scientific Research (A)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Catalyst/Resource chemical process
• Research Institution: Tottori University
• Principal Investigator: MIKI Niwa Tottori University, 大学院・工学研究科, 教授 (10023334)
• Co-Investigator(Kenkyū-buntansha): KATADA Naonobu 鳥取大学, 大学院・工学研究科, 准教授 (00243379) ; OKUMURA Kazu 鳥取大学, 大学院・工学研究科, 助教 (30294341)
• Project Period (FY): 2006 – 2008
• Project Status: Completed (Fiscal Year 2008)
• Budget Amount: ¥31,850,000 (Direct Cost: ¥24,500,000、Indirect Cost: ¥7,350,000); Fiscal Year 2008: ¥7,800,000 (Direct Cost: ¥6,000,000、Indirect Cost: ¥1,800,000); Fiscal Year 2007: ¥12,220,000 (Direct Cost: ¥9,400,000、Indirect Cost: ¥2,820,000); Fiscal Year 2006: ¥11,830,000 (Direct Cost: ¥9,100,000、Indirect Cost: ¥2,730,000)
• Keywords: ゼオライト / 固体酸性質 / 昇温脱離実験 / アンモニア / ブレンステッド酸 / 密度汎関数法計算 / パラフィン分解 / モノレイヤー固体酸酸化物 / IRMS-TPD / ブレーンステッド酸 / 金属酸化物モノレイヤー / 触媒活性 / 昇温脱離法 / ブレーンステッド酸性質 / 金属酸化物 / トルエン吸着

Research Abstract

ゼオライト骨格内に存在する固体酸点の酸量と酸強度を, 個々に測定する新しい測定方法を開発した. 測定した酸強度が密度汎関数法による理論値に一致することをみとめた. この結果, 実験と理論の両面からゼオライト酸性質を解析する総合的な研究方法が得られた. この方法を使うことによって,シャバサイトやYゼオライトに存在する複数のブレンステッド酸点の酸性質, さらに,石油精製などにおいて実際に利用されている修飾Yゼオライト触媒の酸性質を詳しく解析した. 同時に, 酸性質と触媒活性の相関性を考察した.

Research Products

• [Journal Article] Periodic DFT Calculation of the Energy of Ammonia Adsorption on Zeolite Bronsted Acid Sites to Support the Ammonia IRMS-TPD Experiment (2009)
  • Author(s): K. Suzuki, G. Sastre, N. Katada, M. Niwa
  • Journal Title: Chem. Lett. 38 Pages: 354-355
  • NAID: 10025120960
  • Peer Reviewed
• [Journal Article] Periodic Density Functional Calculation on Bronsted Acidity of Modified Y-type Zeolite (2009)
  • Author(s): K. Suzuki, T. Noda, G. Sastre, N. Katada, M. Niwa
  • Journal Title: J.Phys. Chem., C 113 Pages: 5672-5680
  • Peer Reviewed
• [Journal Article] Periodic Density Functional Calculation on Bronsted Acidity of Modified Y-type Zeolite (2009)
  • Author(s): K. Suzuki
  • Journal Title: J. Phys. Chem. C 113 Pages: 5672-5680
  • Peer Reviewed
• [Journal Article] Periodic DFT Calculation of the Energy of Ammonia Adsorption on Zeolite Bronsted Acid Sites to Support the Ammonia IRMS-TPD Experiment (2009)
  • Author(s): K. Suzuki
  • Journal Title: Chem. Lett. 38 Pages: 354-355
  • Peer Reviewed
• [Journal Article] Combined Study of IRMS-TPD Measurement and DFT Calculation on Bronsted Acidity and Catalytic Cracking Activity of Cation Exchanged Y Zeolite (2008)
  • Author(s): T, Noda, K. Suzuki, N. Katada, M. Niwa
  • Journal Title: J. Catal. 259 Pages: 203-210
  • Peer Reviewed
• [Journal Article] Measurements of Number and Strength Distribution of Bronsted and Lewis Acid Sites on Sulfated Zirconia by Ammonia IRMS-TPD Method (2008)
  • Author(s): N. Katada, T. Tsubaki, M. Niwa
  • Journal Title: Appl. Catal., A : General 340 Pages: 76-86
  • Peer Reviewed
• [Journal Article] Acidity and Catalytic Activity of Mesoporous ZSM-5 in Comparison with Zeolite ZSM-5, Al-MCM-41 and Silica-Alumina (2008)
  • Author(s): K. Suzuki, Y. Aoyagi, N. Katada, M. Choi, R. Ryoo, M. Niwa
  • Journal Title: Catal. Today 132 Pages: 38-45
  • Peer Reviewed
• [Journal Article] Acidity and Catalytic Activity of Mesoporous ZSM-5 in Comparison with Zeolite ZSM-5, Al-MCM-41 and Silica-Alumina (2008)
  • Author(s): K. Suzuki
  • Journal Title: Catal. Today 132 Pages: 38-45
  • Peer Reviewed
• [Journal Article] Measurements of Number and Strength Distribution of Bronsted and Lewis Acid Sites on Sulfated Zirconia by Ammonia IRMS-TPD Method (2008)
  • Author(s): N. Katada
  • Journal Title: Appl. Catal. A : General 340 Pages: 76-86
  • Peer Reviewed
• [Journal Article] Combined Study of IRMS-TPD Measurement and DFT Calculation on Bronsted Acidity and Catalytic Cracking Activity of Cation Exchanged Y Zeolite (2008)
  • Author(s): T. Noda
  • Journal Title: J. Catal. 259 Pages: 203-210
  • Peer Reviewed
• [Journal Article] Ammonia IRMS-TPD Measurements and DFT Calculation on Acidic Hydroxyl Groups in CHA-type Zeolites (2007)
  • Author(s): K. Suzuki, G. Sastre, N. Katada, M. Niwa
  • Journal Title: Phys. Chem. Chem. Phys. 9 Pages: 5980-5987
  • Peer Reviewed
• [Journal Article] Quantitative Measurements of Bronsted Acidity of Zeolites by Ammonia IRMS-TPD Method and Density Functional Calculation (2007)
  • Author(s): K. Suzuki, G. Sastre, N. Katada, M. Niwa
  • Journal Title: Chem. Lett. 36 Pages: 1034-1035
  • NAID: 10019844753
  • Peer Reviewed
• [Journal Article] IRMS-TPD of ammonia : Direct and Individual Measurement of Bronsted Acidity in Zeolites and its Relationship with the Catalytic Cracking Activity (2007)
  • Author(s): K. Suzuki, T. Noda, N. Katada, M. Niwa
  • Journal Title: J. Catal. 250 Pages: 151-160
  • Peer Reviewed
• [Journal Article] Detection and Quantitative Measurements of Four Kinds of OH in HY Zeolite (2007)
  • Author(s): K. Suzuki, N. Katada, M. Niwa
  • Journal Title: J. Phys. Chem., C 111 Pages: 894-900
  • Peer Reviewed
• [Journal Article] Detection and Quantitative Measurements of Four Kinds of OH in HY Zeolite (2007)
  • Author(s): K. Suzuki
  • Journal Title: Journal of Physical Chemistry, C 111 Pages: 894-900
  • Peer Reviewed
• [Journal Article] IRMS-TPD of Ammonia: Direct and Individual Measurement of Bronsted Acidity in Zeolites and its Relationship with the Catalytic Cracking Activity (2007)
  • Author(s): K. Suzuki
  • Journal Title: Journal of Catalysis 250 Pages: 151-160
  • Peer Reviewed
• [Journal Article] Quantitative Measurements of Bronsted Acidity of Zeolites by Ammonia IRMS-TPD Method and Density Functional Calculation (2007)
  • Author(s): K. Suzuki
  • Journal Title: Chemistry Letters 36 Pages: 1034-1035
  • Peer Reviewed
• [Journal Article] Ammonia IRMS-TPD Measurements and DFT Calculation on Acidic Hydroxyl Groups in CHA-type Zeolites (2007)
  • Author(s): K. Suzuki
  • Journal Title: Physical Chemistry Chemical Physics 9 Pages: 5980-5987
  • Peer Reviewed
• [Journal Article] Acidity and Catalytic Activity of Mesoporous ZSM-5 in Comparison with Zeolite ZSM-5, A1-MCM-41 and Silica-Alumina (2007)
  • Author(s): K. Suzuki
  • Journal Title: Catalysis Today 132 Pages: 38-45
  • Peer Reviewed
• [Journal Article] Detection and Quantitative Measurements of Four Kinds of OH in HY Zeolite (2007)
  • Author(s): K.Suzuki, N.Katada, M.Niwa
  • Journal Title: Journal of Physical Chemistry, C 111 Pages: 894-900
• [Journal Article] Analysis of Toluene Adsorption on Na-form Zeolite Using Temperature-Programmed Desorption Method (2007)
  • Author(s): R.Yoshimoto, K.Hara, K.Okumura, N.Katada, M.Niwa
  • Journal Title: Journal of Physical Chemistry, C 111 Pages: 1474-1479
• [Journal Article] Identification and Measurements of Strong Bronsted Acid Site in Ultra-Stable Y (USY) Zeolite (2006)
  • Author(s): M. Niwa, K. Suzuki, K. Isamoto, N. Katada
  • Journal Title: J. Phys. Chem. B 110 Pages: 264-269
  • Peer Reviewed
• [Journal Article] Identification and Measurements of Strong Bronsted Acid Site in Ultra-Stable Y (USY) Zeolite (2006)
  • Author(s): M.Niwa, K.Suzuki, K.Isamoto, N.Katada
  • Journal Title: Journal of Physical Chemistry, B 110 Pages: 264-269
• [Presentation] 周期的密度汎関数法計算とアンモニアIRMS-TPD測定による修飾Yゼオライトのブレーンステツド酸性質に関する研究 (2008)
  • Author(s): 鈴木 克生
  • Organizer: 第1 0 2回触媒討論会
  • Place of Presentation: 名古屋大学
  • Year and Date: 2008-09-23
• [Presentation] Combined Study of IRMS-TPD Measurements and DFT Calculation on the Bronsted Acidity and Catalytic Cracking Activity of Cation Exchanged Y Zeolites (2008)
  • Author(s): M. Niwa
  • Organizer: 第14回国際触媒学会(14^<th> International Congress on Catalysis)
  • Place of Presentation: Seoul, Korea
  • Year and Date: 2008-07-15
• [Presentation] 周期的密度汎関数法計算とアンモニアIRMS-TPD測定による修飾Yゼオライトのブレンステッド酸性質に関する研究 (2008)
  • Author(s): 鈴木克生, 野田敬之,German Sastre, 片田直伸, 丹羽盤
  • Organizer: 第102回触媒討論会
  • Place of Presentation: 名古屋
• [Presentation] Combined Study of IRMS-TPD Measurements and DFT Calculation on Bronsted Acidity and Catalytic Cracking Activity of Cation Exchanged Y Zeolite (2008)
  • Author(s): T. Noda, K. Suzuki, N. Katada, M. Niwa
  • Organizer: 14^<th> International Congress on Catalysis
  • Place of Presentation: Seoul
• [Presentation] Combined Study on the Brpnsted Acidity in Cation Exchanged Y Zeolites using IRMS-TPD of Ammonia Measurements and DFT Calculation (2008)
  • Author(s): T. Noda, K. Suzuki, N. Katada, M. Niwa
  • Organizer: ICC 14 Pre-Symposium
  • Place of Presentation: 京都
• [Presentation] アンモニアIRMS-TPD法と密度汎関数法計算によるゼオライト内ブレンステッド酸性質の定量的評価 (2007)
  • Author(s): 鈴木 克生
  • Organizer: 触媒学会, 第100回触媒討論会
  • Place of Presentation: 札幌
  • Year and Date: 2007-09-18
• [Presentation] Direct Measurements of Bronsted Acidity of Y Zeolites by IRMS-TPD of Ammonia and its Relation with the Catalytic Cracking Activity (2007)
  • Author(s): M. Niwa
  • Organizer: 15th International Zeolite Conference
  • Place of Presentation: 北京
  • Year and Date: 2007-08-15
• [Presentation] Quantitative measurements of Bronsted acidity of zeolites by ammonia IRMS-TPD method and density functional calculation (2007)
  • Author(s): K. Suzuki
  • Organizer: 15th International Zeolite Conference
  • Place of Presentation: 北京
  • Year and Date: 2007-08-13
• [Presentation] アンモニアIRMS-TPD法と密度汎関数法計算によるゼオライト内ブレンステッド酸性質の定量的評価 (2007)
  • Author(s): 鈴木克生, German Sastre, 片田直伸 ,丹羽幹
  • Organizer: 第100回触媒討論会
  • Place of Presentation: 北海道
• [Presentation] Direct Measurements of Bronsted Acidity of Y Zeolites by IRMS-TPD of Ammonia and its Relation with the Catalytic Cracking Activity (2007)
  • Author(s): M. Niwa, K. Suzuki, T. Noda, N. Katada
  • Organizer: 15^<th> International Zeolite Conference
  • Place of Presentation: 北京
• [Presentation] アンモニアIRMS-TPD法とDFT計算によるY型ゼオライトの酸性質評価 (2007)
  • Author(s): 鈴木克生, 野田敬之, 片田直伸, 丹羽幹
  • Organizer: 第87回日本化学会春季年会
  • Place of Presentation: 大阪
• [Presentation] アンモニアIRMS-TPD法によるSAPOの酸性質測定 (2006)
  • Author(s): 加藤剛, 鈴木克生, 青柳由香里, 片田直伸, 丹羽幹
  • Organizer: 第22回ゼオライト研究会
  • Place of Presentation: 東京
• [Presentation] Brousted Acidity in HY and USY Studied by IRMS-TPD of Ammonia (2006)
  • Author(s): M. Niwa, K. Suzuki, N. Katada
  • Organizer: 16^<th> Saudi Arabia-Japan Joint Symposium
  • Place of Presentation: Dharan
• [Presentation] アンモニアIRMS-TPD法によるinsituHYゼオライトの酸性質測定 (2006)
  • Author(s): 鈴木克生, 片田直伸, 丹羽幹
  • Organizer: 第98回触媒討論会
  • Place of Presentation: 富山