1997 Fiscal Year Annual Research Report

放射性^<35>S及び^3Hパルストレーサー法の開発-硫化物触媒上での硫黄及び水素の挙動の解析

Research Project

Project/Area Number	08455371
Research Institution	Tokyo University of Agriculture and Technology
Principal Investigator	加部利明東京農工大学, 工学部, 教授 (50092482)
Co-Investigator(Kenkyū-buntansha)	神戸正純東京農工大学, 工学部, 助手 (80262244) 石原篤東京農工大学, 工学部, 助教授 (60212908)
Keywords	放射性トレーサー法 / 水素化脱硫反応 / 硫黄挙動の定量 / 水素挙動の定量 / 移動可能な硫黄 / 硫化物触媒構造 / 脱硫反応機構 / 軽油深度脱硫
Research Abstract	この報告書は、平成8年度と9年度の二年間にわたり、文部省科学研究補助金基盤研究(B)(2)(研究課題番号08455371)により、軽油の深度脱硫等石油精製プロセスの中心となる高性能硫化物触媒の開発のため^<35>S及び^3Hパルストレーサー法を用いた硫化物触媒の構造及び脱硫反応機構の解明における研究を行った結果をまとめたものである。硫化物触媒の構造や反応機構の解析は、これまでに各種機器分析及び反応速度の解析により行われてきたが、これらの方法では高温高圧反応下での硫黄の挙動を定量的にとらえることは困難であった。一方、放射性同位体元素^<35>Sトレーサー法の最大の特長は硫化物触媒の高圧下における反応に関与する硫黄の量とその移動性を定量的に測定でき、触媒構造及び反応機構を同時に明らかにできることにある。さらにパルストレーサー法では^<32>Sと^<35>Sトレーサーを容易に切り替えながら反応を行うので、触媒上の硫黄の化学的な挙動を全く変えることなく操作を行え、触媒反応に関与している(移動可能な)硫黄量とその移動速度を定量できる。また、^<35>Sパルストレーサー法で得たノウハウを生かし、このシステムに^3Hパルストレーサー法を導入し、作動状態での触媒上の水素の挙動を定量できる。本研究では、軽油の深度脱硫でも注目されるモリブデン系硫化物触媒に着目し、作動状態の脱硫触媒上における硫黄と水素の挙動を同時に定量し、水素化脱硫触媒の構造及び脱硫反応機構を解明したもので、従来の研究には見られない多くの新しい知見を見出し、深度脱硫に対応する触媒の開発の指針となる結果を提供しているものである。

Research Products

(15 results)

All Other

All Publications (15 results)

[Publications] Q.zhang: "Deep Desulfurization of Light oil.4.Hydrodesulf urization of Methy-substituted Diben zothiophenes Catalyzed by various Co-Mo/Al_2O_3 and Mi-Mo/Al_2O_3 Catnlyses" Sekiyu Gakkaishi. 39. 410-417 (1996)
[Publications] T.Kabe: "Sulfur exchange on CoMo/Al_2O_3 hydrodesulfurization Catalyst using ^<35>S radioisotope tracer" Catal. Today. 29. 197-202 (1996)
[Publications] A.Ishihara: "(Part4) Hydrodesulfurization Catalysts prepared from alumina and Silica-alumina supported molybdcnum and cobalt carbonyls" Sekiyu Gakkaishi. 39. 26-33 (1996)
[Publications] A.Ishihara: "Part5 Catalysts for hydrodesulfurization prepared from alumina-supported nothenium Carbonyl-alkali metal hydroxide system" Sekiyu Gakkaishi. 39. 211-221 (1996)
[Publications] A.Ishihara: "Part6 effect of supports on activities of HDS Catalysts prepared from supported ruthenium carbonyl-Cesium hydroxide systems" Sekiyu Gakkaishi. 39. 403-409 (1996)
[Publications] T.Kabe: "Sulfidation of molybdenium-based alumina Catalysts using a radioisotope tracer method" J.Chem. Soc.Faraday trans. 93. 3709-3713 (1997)
[Publications] A.Ishihara: "Elucidation of Sulfur Bcluir on Alumina-supported Ruthenium sulfide-cosium Catalyets using Radioactive ^<35>S as a Traces" Chem.Lett. 743-744 (1996)
[Publications] Q.zhang: "The role of Cabalt of Hydrodesulfurization and Hydrogenation of Diben20t nline and 4,6-Dimethyldiben20thiophene Cataly2ed by Co-Mo/Al_2O" J.Jpn. Petrol.Inst.(Sekiyu Gakkaishi). 40. 408-414 (1997)
[Publications] Q.zhang: "Effect of ths on Hydrodesulfurization of Diben 20 thiophene and 4.6-Dimethyl diben20thiophene" J.Jpn.Petiol.Insi (Sekiyu Gakkaishi). 40. 185-191 (1997)
[Publications] T.Kabe: "Elucideition of Hydrodesulfurization Mechanism Using ^<35>S Radioisotope Pulse Tracer Methods" Catalysis Today. 1107. 1-10 (1997)
[Publications] W.Qian: "Elucidation of Molybdenum-based Catalysts Using a Radioisotope Tracer Method (Part1) Hydrodesulfurization Activitly and siucture of Sulfided Molybdena-Alumina Cal" J.Chem.Soc.Faraday Trans. 93. 1821-1826 (1997)
[Publications] W.Qian: "(Part2) Promotion Effect of Cobalt for Molybdena-Alumina catalysts" J.Chem.Soc.Faraday Trans. 93. 4395-4400 (1997)
[Publications] W.Qian: "Elucidation of Bchanior of sulfur on sulfided CO-MO/Al_2O_3 Catalysts using a ^<35>S Radioisotope pulse Tracer Method" J.Catal. 170. 286-294 (1997)
[Publications] Q.Zhang: "(Part5) Hydrodesulfarization of Methy-subsrituted Banzothiopenes and Dibenzo-phene in Light gas oil Catalyzed by various sulfided CO-MO/Al_2O_3 and Nl-MO/Al_2O_3 Catalysts" J.Jpn.Petrol.Ict (Sekiyu Gakkaishi). 40. 29-34 (1997)
[Publications] A.Ishihara: "(Part7) Hydrodesulturization Catalysts prepared from Alumina-supported Ruthenium Carbonyh-Alkaline-earth Metal Hydroxide system" J.Jpn.Petrol.Inst (Sekiyu Gakkaishi). 40. 516-523 (1997)

1997 Fiscal Year Annual Research Report

放射性^<35>S及び^3Hパルストレーサー法の開発-硫化物触媒上での硫黄及び水素の挙動の解析

Principal Investigator

加部 利明 東京農工大学, 工学部, 教授 (50092482)

Research Products

[Publications] Q.zhang: "Deep Desulfurization of Light oil.4.Hydrodesulf urization of Methy-substituted Diben zothiophenes Catalyzed by various Co-Mo/Al_2O_3 and Mi-Mo/Al_2O_3 Catnlyses" Sekiyu Gakkaishi. 39. 410-417 (1996)

[Publications] T.Kabe: "Sulfur exchange on CoMo/Al_2O_3 hydrodesulfurization Catalyst using ^<35>S radioisotope tracer" Catal. Today. 29. 197-202 (1996)

[Publications] A.Ishihara: "(Part4) Hydrodesulfurization Catalysts prepared from alumina and Silica-alumina supported molybdcnum and cobalt carbonyls" Sekiyu Gakkaishi. 39. 26-33 (1996)

[Publications] A.Ishihara: "Part5 Catalysts for hydrodesulfurization prepared from alumina-supported nothenium Carbonyl-alkali metal hydroxide system" Sekiyu Gakkaishi. 39. 211-221 (1996)

[Publications] A.Ishihara: "Part6 effect of supports on activities of HDS Catalysts prepared from supported ruthenium carbonyl-Cesium hydroxide systems" Sekiyu Gakkaishi. 39. 403-409 (1996)

[Publications] T.Kabe: "Sulfidation of molybdenium-based alumina Catalysts using a radioisotope tracer method" J.Chem. Soc.Faraday trans. 93. 3709-3713 (1997)

[Publications] A.Ishihara: "Elucidation of Sulfur Bcluir on Alumina-supported Ruthenium sulfide-cosium Catalyets using Radioactive ^<35>S as a Traces" Chem.Lett. 743-744 (1996)

[Publications] Q.zhang: "The role of Cabalt of Hydrodesulfurization and Hydrogenation of Diben20t nline and 4,6-Dimethyldiben20thiophene Cataly2ed by Co-Mo/Al_2O" J.Jpn. Petrol.Inst.(Sekiyu Gakkaishi). 40. 408-414 (1997)

[Publications] Q.zhang: "Effect of ths on Hydrodesulfurization of Diben 20 thiophene and 4.6-Dimethyl diben20thiophene" J.Jpn.Petiol.Insi (Sekiyu Gakkaishi). 40. 185-191 (1997)

[Publications] T.Kabe: "Elucideition of Hydrodesulfurization Mechanism Using ^<35>S Radioisotope Pulse Tracer Methods" Catalysis Today. 1107. 1-10 (1997)

[Publications] W.Qian: "Elucidation of Molybdenum-based Catalysts Using a Radioisotope Tracer Method (Part1) Hydrodesulfurization Activitly and siucture of Sulfided Molybdena-Alumina Cal" J.Chem.Soc.Faraday Trans. 93. 1821-1826 (1997)

[Publications] W.Qian: "(Part2) Promotion Effect of Cobalt for Molybdena-Alumina catalysts" J.Chem.Soc.Faraday Trans. 93. 4395-4400 (1997)

[Publications] W.Qian: "Elucidation of Bchanior of sulfur on sulfided CO-MO/Al_2O_3 Catalysts using a ^<35>S Radioisotope pulse Tracer Method" J.Catal. 170. 286-294 (1997)

[Publications] Q.Zhang: "(Part5) Hydrodesulfarization of Methy-subsrituted Banzothiopenes and Dibenzo-phene in Light gas oil Catalyzed by various sulfided CO-MO/Al_2O_3 and Nl-MO/Al_2O_3 Catalysts" J.Jpn.Petrol.Ict (Sekiyu Gakkaishi). 40. 29-34 (1997)

[Publications] A.Ishihara: "(Part7) Hydrodesulturization Catalysts prepared from Alumina-supported Ruthenium Carbonyh-Alkaline-earth Metal Hydroxide system" J.Jpn.Petrol.Inst (Sekiyu Gakkaishi). 40. 516-523 (1997)

加部利明東京農工大学, 工学部, 教授 (50092482)