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이익춘,이재의,정대형,Ikchoon Lee,Jae Eui Yie,Dae Hyung Chung Korean Chemical Society 1976 대한화학회지 Vol.20 No.1
염화벤젠술페닐의 바람직한 형태를 EHMO법으로 구하였다. 이 형태의 안정도는 황원자와 벤젠고리 사이의 n-${\pi}$ 콘쥬게이션에 따른다는 것을 알았다. 또 염화벤젠술페닐의 가에탄올 분해반응을 연구하여 얻은 반응속도상수를 치환기 효과와 황원자의 d-궤도함수 기여로 논의하였다. 비선형 Hammett 그래프로 부터 쌍뿔형의 중간체를 제안할 수 있었다. The preferred conformation of benzenesulfenyl chloride was determined by EHMO calculation. It was found that the stability was dictated by the n-${\pi}$ conjugation of S atom with the benzene ring. The ethanolysis reaction of benzenesulfenyl chlorides has been studied. The rate constants obtained have been discussed in terms of substituent effects and d-orbital participation of sulfur atom. From a non-linear Hammett plot, bipyramid type of intermediate has been suggested.
김영길,이재의,조성준,유룡 ( Young Kil Kim,Jae Eui Yie,Sung June Cho,Ryong Ryoo ) 한국공업화학회 1994 공업화학 Vol.5 No.5
Ru/γ-Al₂O₃와 Ru/CeO₂-γ-Al₂O₃를 사용하여 Ru담지 촉매의 반응성과 열적노화현상에 미치는 Ce의 영향을 연구하였다. ^(129)Xe-NMR과 수소흡착법을 사용하여 촉매특성을 검토하였으며, 모사 자동차 배기가스를 사용하여 과농, 양론 및 희박조건에서의 CO, HC 및 NO_x 전환율을 측정하였다. 새촉매와 노화촉매 모두 Ru/CeO₂-γ-Al₂O₃가 Ru/γ-Al₂O₃보다 세 가지 오염물질에 대한 전환율이 높았다. ^(129)Xe-NMR과 수소흡착에 의하면 Ce을 첨가하여도 열적노화현상을 억제할 수 없었다. 그러나 673K에서 열적노화시킨 경우 Ru/γ-Al₂O₃의 반응성은 새 촉매보다 작았으나 Ru/CeO₂-γ-Al₂O₃의 반응성은 오히려 컸다. 이것은 열적 노화과정에서 Ru/Ce 사이의 계면에 아마도 새로운 활성점이 만들어지기 때문이 아닌가 사료된다. 또한, Ru금속에 미치는 Ce같은 양이온 효과를 좀더 정량적으로 구하기 위하여 Ca, Ba, La, Y, Ce 등의 양이온을 교환한 Y-제올라이트에 Ru을 담지시킨 모델 촉매의 열적노화 정도를 ^(129)Xe-NMR과 EXAFS로 연구한 결과 이들 양이온이 Ru의 열적 노화성에 거의 영향을 미치지 못하는 것을 관찰하였다. Effects of ceria additive on the activity and thermal aging behavior of supported Ru catalysts were investigated using Ru/γ-Al₂O₃ and Ru/CeO₂-γ-Al₂O₃. The catalysts were characterized by ^(129)Xe-NMR and H₂ chemisorption. The cataltic activity for conversion of CO, HC and NO_x was measured using simulated automobile engine exhausts under lean, rich and stoichiometric conditions. For both fresh and aged catalysts, Ru/CeO₂-γ-Al₂O₃ was more active than Ru/γ-Al₂O₃ for all three pollutants. Results of 129 Xe-NMR and H₂ chemisorption indicated that sintering of Ru particles occurred to the same extent for both catalysts during the thermal aging process. After thermal aging at 673K, however, the catalytic activity of the aged Ru/CeO₂-γ-Al₂O₃ was substantially higher than that of the fresh one, while the activity of Ru/γ-Al₂O₃ decreased after the thermal aging. This finding may suggest new active sites were created during the thermal aging, probably in the vicinity of the interface between Ru and Ce. For more quantitative investigation of the effect of a cation such as Ce on the thermal aging of Ru metal particles, Ru catalysts supported on cation-exchanged Y-zeolites were used as the model catalysts. The results indicated that when Ba, Ca, La, Y or Ce was used for the canon exchange, the exchanged cation did not affect the thermal aging behavior of Ru in Y-zeolite, as evidenced by ^(129)Xe-NMR and EXAFS.
Pt - Rh 이원금속 촉매의 구조와반응성에 관한 연구
김영길,신기환,이재의 ( Young Kil Kim,Ki Whan Shin,Jae Eui Yie ) 한국공업화학회 1996 공업화학 Vol.7 No.4
NaY 제올라이트에 Pt/Rh비를 달리하여 이온교환법으로 제조한 Pt-Rh촉매의 특성을 ^(129)Xe-NMR과 EXAFS 방법으로 특성조사를 하였다. ^(129)Xe-NMR과 EXAFS 자료는 PtRh 이원금속 클러스터의 표면으로 Rh 원자들이 모이는 것으로 나타났다. 모사 자동차 배기가스를 사용하여 희박, 과농 및 양론조건에서 CO, HC 및 NO_x 전환율을 측정하였으며, Pt-Rh/NaY(Pt/Rh=1) 이원금속 촉매가 다른 촉매들보다 세가지 오염물질에 대한 반응활성이 높게 나타남을 알 수 있었다. Pt-Rh/NaY catalysts with various Pt/Rh ratios were prepared by an ion-exchange method and their characteristics were investigated by ^(129)Xe-NMR and EXAFS. Both the ^(129)Xe-NMR and EXAFS data indicate that the surface of PtRh bimetallic clusters was enriched with Rh atoms. The catalytic activities of these catalysts for conversion of CO, HC and NO_x were measured by using simulated automobile engine exhausts under lean, rich and stoichiometric conditions. The Pt-Rh/NaY(Pt/Rh=1) catalyst exhibited the greatest reactive activity among the catalysts used in this study.
윤기준,정경숙,이재의 ( Ki June Yoon,Kyeong Sug Jeong,Jae Eui Yie ) 한국화학공학회 1993 Korean Chemical Engineering Research(HWAHAK KONGHA Vol.31 No.5
Decomposition of methanol over a Ni/SiO₂ catalyst was carried out using a tubular flow reactor in a temperature range between 473 and 533 K. The partial pressure of methanol was below 0.141 atm. H₂ and CO were the major decomposition products, and a small amount of CH₄ was produced. Although the amount of CH₄ formed increased with temperature, the selectivity to CO was greater than 95%. The following rate equation was proposed and the kinetic parameter values were evaluated. -r_A=k_s K_A P_A/(1+K_A P_A)²
이원금속 촉매의 접촉개질 반응 성능 연구 - 1. Pt-Mo 이원금속의 특성과 반응성
김영길(Young Kil Kim),연태헌(Tae Hun Yeon),유룡(Ryong Ryoo),이재의(Jae Eui Yie) 한국화학공학회 1997 Korean Chemical Engineering Research(HWAHAK KONGHA Vol.35 No.1
The formation of Pt-Mo bimetallic clusters on γ-Al₂O₃ has been investigated using magic angle spinning ^(27)Al NMR spectroscopy. ^(129)Xe NMR spectroscopy, transmission electron microscopy, hydrogen chemisorption and catalytic dehydrocyclization of n-hexane. The chemical shift in ^(129)Xe NMR for the Pt-Mo/γ-Al₂O₃ system decreased with the addition of Mo, indicating the formation of Pt-Mo bimetallic clusters. The formation of the bimetallic clusters with the addition of 0.1-0.5 wt% Mo to 1 wt% Pt/γ-Al₂O₃ led to a remarkable decrease in the catalytic activity, probably due to the Pt atoms being masked physically by the Mo atoms located on the surface of the Pt particles. On the contrary, the catalytic activity increased significantly when 0.01 wt% Mo was added. The small quantity of Mo seemed to he located at the Pt-alumina interface, stabilizing the cluster by anchoring to the support. Electronic effects due to the Mo addition may also be suggested to enhance the activity.