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- 학위논문
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- 지도교수
- 이영우, 걍용
- 발행연도
- 2020
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For the reaction of formaldehyde vapor, Heteropoly acid catalysts were supported carbon with various composition of phosphoric acid(H_(3)PO_(4)), vanadium(Ⅴ) pentoxide(V_(2)O_(5)) and molybdenum(Ⅵ) trioxide(MoO_(3)). Catalytic performance was examined at 140 ℃ for 1hour in vapor formaldehyde. The prepared catalysts were characterized by ICP-OES, XRD, BET and DRIFTS. Acidity of the catalysts was investigated with NH_(3)-TPD and Pyridine-DRIFTS.
Formaldehyde conversion of the catalysts was increased with decreasing the composition of Mo and P and increasing that of V. As a result of specific surface area and XRD analysis, it was considered that small particles of heteropoly acid phase and oxides of Mo and V were evenly distributed on the activated carbon support maintaining large specific surface area. The DRIFTS analysis of the catalysts showed the presence of Keggin structure in heteropoly acid phase which was highly developed in the P_(1)V_(0.5)Mo_(10)/AC catalyst.
In NH_(3)-TPD results, it was found that three types of acid sites in the acidic strength existed on the catalysts, where the ratio of the acid site having the strong strength was linear relationship to the formaldehyde conversion. As the conversion of formaldehyde could be affected by the Mo/V molar ratio, it was worth noting that the acidity of the catalysts would be adjusted by the Mo/V molar ratio. The spectra of pyridine-DRIFTS exhibited that the acid sites of catalysts were mostly present in a Lewis form rather than a Bronsted one. The decrease of Lewis acid could enhance the composition of the strong acid sites.
Therefore, it was concluded that the reactivity of the heteropoly acid catalysts to formaldehyde could be significantly influenced by the amount and acidity of the Lewis acid sites in the catalysts, which would be controlled by the molar ratio of Mo and V components supported on activated carbon.
Formaldehyde conversion of the catalysts was increased with decreasing the composition of Mo and P and increasing that of V. As a result of specific surface area and XRD analysis, it was considered that small particles of heteropoly acid phase and oxides of Mo and V were evenly distributed on the activated carbon support maintaining large specific surface area. The DRIFTS analysis of the catalysts showed the presence of Keggin structure in heteropoly acid phase which was highly developed in the P_(1)V_(0.5)Mo_(10)/AC catalyst.
In NH_(3)-TPD results, it was found that three types of acid sites in the acidic strength existed on the catalysts, where the ratio of the acid site having the strong strength was linear relationship to the formaldehyde conversion. As the conversion of formaldehyde could be affected by the Mo/V molar ratio, it was worth noting that the acidity of the catalysts would be adjusted by the Mo/V molar ratio. The spectra of pyridine-DRIFTS exhibited that the acid sites of catalysts were mostly present in a Lewis form rather than a Bronsted one. The decrease of Lewis acid could enhance the composition of the strong acid sites.
Therefore, it was concluded that the reactivity of the heteropoly acid catalysts to formaldehyde could be significantly influenced by the amount and acidity of the Lewis acid sites in the catalysts, which would be controlled by the molar ratio of Mo and V components supported on activated carbon.
목차
1. 서 론 ·································································································································································12. 이론적 고찰 ·······················································································································································42.1. 포름알데히드의 반응 ·······································································································································42.2. 촉매의 구성 ····················································································································································72.2.1. Heteropoly aicd 및 PVMo 촉매 ···················································································································72.2.2. 활성탄 지지체 ············································································································································123. 실 험 ·······························································································································································153.1. 촉매 제조 ·····················································································································································153.2. 촉매 반응성 실험 ···········································································································································173.3. 촉매 특성 분석 ··············································································································································193.3.1. ICP-OES (Inductively Coupled Plasma Optical Emission Spectrometer) ···················································193.3.2. BET (Brunauer, Emmett, Teller) ···············································································································193.3.3. XRD (X-Ray Diffraction) ···························································································································193.3.4. DRIFTS (Diffuse Reflectance Infrared Fourier Transform Spectroscopy) ··················································203.4. 촉매 산점 분석 ··············································································································································203.4.1. NH_(3)-TPD (Temperature Programmed Desorption of Ammonia) ····························································203.4.2. Pyridine-DRIFTS (Pyridine-Diffuse Reflectance Infrared Fourier Transform Spectroscopy) ·······················214. 결과 및 고찰 ····················································································································································224.1. 촉매 반응성 ··················································································································································224.2. 촉매 특성 분석 ··············································································································································294.2.1. ICP-OES ···················································································································································294.2.2. BET ··························································································································································324.2.3. XRD ·························································································································································344.2.4. DRIFTS ·····················································································································································394.3. 촉매 산점 분석 ··············································································································································504.3.1. NH_(3)-TPD ·················································································································································504.3.2. Pyridine-DRIFTS ·······································································································································585. 결론 ································································································································································63참고문헌 ······························································································································································65ABSTRCT * ·························································································································································75
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