[국가R&D연구보고서]나노 기술 기반 폐글리세롤 및 폐락틱산/숙신산 활용 고부가가치 바이오 화합물 제조 촉매 기술 및 공정 개발 Process Development for Production of high-valued bio-chemicals From Waste Biomass원문보기
연구개발결과 ◦ 글리세롤로부터 1,2-프로판디올, 1,3-프로판디올, 폴리우레탄 및 아크릴산 직접 생산기술 개발 - 고온/고압 반응기 설계 및 제조 - 구리 담지 촉매에 의한 1,2-프로판디올 생산과 조촉매의 첨가로 90%이상의 수율달성 - 글리세롤로부터 1,3-프로판디올 생산을 위한 귀금속(Pt) 담지 촉매의 경우 최고 성능 확인 (55.6% 수율) - PCL (polycaprolactone)을 사용하여 기존에 쉽게 깨지는 성질을 보완하여 유연한 폴리우레탄을 합성함. - 3차원의 열린 중형 기공 구
연구개발결과 ◦ 글리세롤로부터 1,2-프로판디올, 1,3-프로판디올, 폴리우레탄 및 아크릴산 직접 생산기술 개발 - 고온/고압 반응기 설계 및 제조 - 구리 담지 촉매에 의한 1,2-프로판디올 생산과 조촉매의 첨가로 90%이상의 수율달성 - 글리세롤로부터 1,3-프로판디올 생산을 위한 귀금속(Pt) 담지 촉매의 경우 최고 성능 확인 (55.6% 수율) - PCL (polycaprolactone)을 사용하여 기존에 쉽게 깨지는 성질을 보완하여 유연한 폴리우레탄을 합성함. - 3차원의 열린 중형 기공 구조를 갖는 산 촉매 물질을 제조하여 기존의 상용 산 촉매(HZSM-5, MCM-41)와 비교하여 우수한 활성과 높은 안정성을 나타냄 - 일정한 구조를 유지하면서 산 특성을 조절 할 수 있는 특징을 가져 응용가능성이 높음 - 산 촉매와 산화 촉매의 이중층 촉매 시스템을 통해 글리세롤로부터 아크릴산을 생산함. 특히, 이번 연구에서 새로 개발된 촉매와 몰리브데늄-바나듐의 혼합산화물 촉매를 이용하여 40%이상의 아크릴산 수율을 얻음. - 정제하지 않은 글리세롤을 반응물을 사용하여 테스트를 진행하였음. - 이원기능촉매 개발을 통하여 한 촉매 하에서 아크릴산 직접 생산 가능. - 벤치 규모에서의 아크릴산 생산을 위해 산 촉매와 산화 촉매를 성형함. 스케일업 후에도 40 % 이상의 아크릴산 수율 달성. - 산 촉매와 산화 촉매의 이중층 반응 시스템에서 반응 속도론적 연구를 기반으로 하여 반응 속도 파라미터를 계산함. 이를 통해 글리세롤로부터 아크릴산을 생산하는 공정의 설계, 모사 및 유용성평가. - 실제 폐글리세롤을 40 %의 수율로 아크릴산 전환에 성공함. ◦ 폐락틱산/폐숙신산 전환 연구 - 고온, 고압 분위기에 일어나는 폐락틱산의 수소화분해 반응을 위해 회분식 반응기를 설계 - 금속스크리닝을 통하여 루테늄 담지 촉매의 높은 활성 및 프로필렌글리콜의 선택도 확인 - 반응 장치 설계 및 반응 실험 조건 확립 - 팔라듐(Pd) 담지 촉매에서의 반응 온도와 압력에 따른 감마부티로락톤의 수율 변화를 확인. 알루미나 제어로젤에 담지된 촉매가 상용 알루미나에 담지된 촉매에 비해 우수한 활성을 보임. - 팔라듐(Pd)-알루미나 복합체 촉매를 제조 후 폐숙신산의 수소화 반응에 응용함. - 레늄(Re)과 구리(Cu)가 포함된 탄소복합체 촉매를 이용하여 벤치규모의 실증화를 달성함. 레늄이 포함된 촉매가 재이용성과 안정성에서 더 우수함을 보임.
Abstract▼
Ⅳ. Results ◦ Development of metal supported catalysts to produce 1,2-PDO and 1,3-PDO from glycerol - Design of reactor for high T, P conditions - Glycerol was converted into 1,2-PDO over Cu-supported catalysts and effects of promoters such as Cr were studied. Over Pt-supported catalysts the
Ⅳ. Results ◦ Development of metal supported catalysts to produce 1,2-PDO and 1,3-PDO from glycerol - Design of reactor for high T, P conditions - Glycerol was converted into 1,2-PDO over Cu-supported catalysts and effects of promoters such as Cr were studied. Over Pt-supported catalysts the highest yield (55.6%) for 1,3-PDO was achieved. ◦ Synthesis of polyurethane exploiting polyols derived from glycerol - MDI (Methylene diphenyl diisocyanate diisocyanate) and HDI (Hexamethylene diisocyanate) were used to synthesize polyurethane from polyols derived from glycerol. The more flexible polyurethane were synthesized by using PCL (polycaprolactone) to cover its fragile property. ◦ Preparation of nano-structured acid catalysts(DAS, DASP) for glycerol dehydration and elucidation on effects of catalytic properties on the reaction - Development of 3D mesoporous acid catalysts. Compared to typical acid catalysts such as HZSM-5 and MCM-41, the developed catalysts showed high catalytic performance and stability. - Due to the uniform structure and tuneable acidic properties, the developed catalysts are expected to applicable to various reactions. ◦ Production of acrylic acid from glycerol on the two bed catalytic system - Acrylic acid were produced from glycerol over the catalyst bed consisting of acid catalyst and oxidative catalyst. Over DASP and Mo-V oxide catalysts, glycerol afforded acrylic acid in more than 40% yield. ◦ Direct conversion of glycerol into acrylic acid over bifunctional catalyst - Preparation of Mo-V-W based catalysts to convert glycerol into acrylic acid directly. The bifunctional catalyst make it possible to simplify the reactor system. ◦ Design of reaction system and optimization of reaction condition - Batch reactor system was used for hydrogenolysis of lactic acid under high T, P conditions ◦ Development of efficient catalysts to produce propylene glycol via dehydration of lactic acid - Metal supported catalysts were prepared and test to convert lactic acid into propylene glycero. Among various metal, Ru was the most active material for the reaction. - The effects of support materials were studied. ◦ Design of batch reactor system for conversion of succinic acid reactions - Installation of batch reactor system for high T, P conditions ◦ Screening and preparation of catalytic materials for conversion of succinic acid into any desired products. - Over Pd supported catalysts, effects of reaction condition(T, P) on yields for γ-butyrolactone were studied. Pd catalysts using alumina Xerogel showed more enhanced catalytic activity than typical alumina support. - Pd-Alumina composite catalysts were prepared and applied to hydrogenation of succinic acid. ◦ Scale up of the reaction system producing acrylic acid from glycerol - Extrusion of acid catalysts and coating of oxidative catalysts were preceded and the reactor system was scaled up. Based on the results of bench-scaled reaction tests, catalytic performance was evaluated. ◦ Evaluation of product distribution and catalytic performance at a bench-scaled reactor ◦ Process simulation of acrylic acid production from glycerol based on kinetic studies - Based on kinetic studies, kinetic parameters for the reactions to produce acrylic acid from glycerol were estimated. The process producing acrylic acid from glycerol was designed and the kinetic parameters were applied to reflect catalytic performance in the simulating software. ◦ Scale up of succinic acid conversion process - Re- and Cu-Carbon composite catalysts were used in the bench-scaled reaction tests. The former catalysts showed better catalytic performance in terms of reneration and stability.
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