금속산화물 촉매상에서 플라즈마를 이용한 IPA 저감 = Plasma-assisted Catalysis for the Abatement of Isopropyl Alcohol over Metal Oxides

국문 초록 (Abstract)

금속산화물이 담지된 허니컴 형상의 플라즈마-촉매 반응기를 이용하여 아이소프로필 알코올(isopropyl alcohol, IPA) 저감 및부산물 생성 거동에 대해 조사하였다. 허니컴 형상의 다공질 세라믹 지지체(주성분: α-Al2O3)에 금속산화물로 산화철(Fe2O3)또는 산화구리(CuO)를 담지시킨 후, 이 촉매가 동축 원통형 전극구조 내부에 위치하도록 플라즈마-촉매 반응기를 구성하였다. 플라즈마 반응에 의한 IPA 분해속도가 매우 빨랐기 때문에 IPA 분해효율 자체는 금속산화물 담지 여부 및 금속산화물 종류에 관계없이 유사한 것으로 나타났으나, 부산물 생성거동은 촉매종류에 따라 큰 차이를 보여주었다. 아세톤, 폼알데하이드,아세트알데하이드, 메테인, 일산화탄소 등의 유해 부산물 농도는 Fe2O3/α-Al2O3 < CuO/α-Al2O3 < α-Al2O3 순으로 높게 나타났다. 유량 1 L min-1, IPA 초기농도 5,000 ppm(산소: 10%), 방전전력 47 W의 조건에서 얻어진 CO2 선택도는 α-Al2O3,CuO/α-Al2O3, Fe2O3/α-Al2O3에 대해 각각 40, 80, 95%로서 Fe2O3/α-Al2O3가 플라즈마-촉매를 이용한 IPA의 산화에 가장 효과적인 것으로 나타났다. 플라즈마를 단독으로 사용하여 휘발성유기화합물을 분해할 경우 타르형태의 생성물이 반응기에퇴적되는 문제점이 있으나, 플라즈마-촉매 공정에서는 이러한 현상이 관찰되지 않았으며 촉매의 활성이 그대로 유지되었다.

다국어 초록 (Multilingual Abstract)

This work investigated the plasma-catalytic decomposition of isopropyl alcohol (IPA) and the behavior of thebyproduct compounds over monolith-supported metal oxide catalysts. Iron oxide (Fe2O3) or copper oxide (CuO) was loaded on amonolithic porous α-Al2O3 support, which was placed inside the coaxial electrodes of plasma reactor. The IPA decompositionefficiency itself hardly depended on the presence and type of metal oxides because the rate of plasma-induced decomposition wasso fast, but the behavior of byproduct formation was largely affected by them. The concentrations of the unwanted byproducts,including acetone, formaldehyde, acetaldehyde, methane, carbon monoxide, etc., were in order of Fe2O3/α-Al2O3 < CuO/α-Al2O3< α-Al2O3 from low to high. Under the condition (flow rate: 1 L min-1; IPA concentration: 5,000 ppm; O2 content: 10%; dischargepower: 47 W), the selectivity towards CO2 was about 40, 80 and 95% for α-Al2O3, CuO/α-Al2O3 and Fe2O3/α-Al2O3, respectively,indicating that Fe2O3/α-Al2O3 is the most effective for plasma-catalytic oxidation of IPA. Unlike plasma-alone processes in whichtar-like products formed from volatile organic compounds are deposited, the present plasma-catalyst hybrid system did not exhibitsuch a phenomenon, thus retaining the original catalytic activity.

참고문헌 (Reference)

1 정원영, "다양한 방법으로 제조된 CuO/CeO2 촉매에서의 벤젠의 연소반응" 한국청정기술학회 19 (19): 128-133, 2013

2 Picasso, G., "Total Combustion of Methyl-Ethyl Ketone over Fe2O3 Based Catalytic Membrane Reactors" 46 : 133-143, 2003

3 Wang, H., "Removal of Four Kinds of Volatile Organic Compounds Mixture in Air Using Silent Discharge Reactor Driven by Bipolar Pulsed Power" 67 : 547-553, 2009

4 Jarrige J., "Plasma-enhanced Catalysis of Propane and Isopropyl Alcohol at Ambient Temperature on a MnO2-based Catalyst" 90 : 74-82, 2009

5 Trinh, H. Q., "Plasma-Catalytic Oxidation of Acetone in Annular Porous Monolithic Ceramic-Supported Catalysts" 251 : 199-206, 2014

6 Jo, J. -O., "Plasma-Catalytic Ceramic Membrane Reactor for Volatile Organic Compound Control," 41 : 3021-3029, 2013

7 Barakat, C., "Oxidation of Isopropanol and Acetone Adsorbed on TiO2 Under Plasma Generated Ozone Flow: Gas Phase and Adsorbed Species Monitoring" 147 : 302-313, 2014

8 Leclercq, J., "Novel Inductively-Heated Catalytic System for Fast VOCs Abatement, Application to IPA in Air" 146 : 131-137, 2014

9 Vandenbroucke, A. M., "Non-thermal Plasmas for Non-catalytic and Catalytic VOC Abatement" 195 : 30-54, 2011

10 L. Sivachandiran, "Isopropanol saturated TiO2 surface regeneration by nonthermal plasma: Influence of air relative humidity" 214 : 17-26, 2013

11 Sivachandiran, L., "Isopropanol Saturated TiO2 Surface Regeneration by Nonthermal Plasma: Influence of Air Relative Humidity" 214 : 17-26, 2013

12 Yamamoto, S., "Investigation of Transition Metal Oxide Catalysts for Diesel PM Removal Under Plasma Discharge Conditions" 1 : 11-16, 2008

13 Schmidt-Szałowski, K., "Hybrid Plasma-Catalytic Systems for Converting Substances of High Stability, Greenhouse Gases and VOC" 89 : 2643-2651, 2011

14 Chen, H., "Fabrication of Porous Copper/Manganese Binary Oxides Modified ZSM-5 Membrane Catalyst and Potential Application in the Removal of VOCs" 254 : 133-142, 2014

15 Jarrige, J., "Decomposition of Three Volatile Organic Compounds by Nanosecond Pulsed Corona Discharge:Study of By-product Formation and Influence of High Voltage Pulse Parameters" 99 : 113-303, 2006

16 Medina-Valtierra, J., "Complete Oxidation of Isopropanol over Cu4O3 (Paramelaconite) Coating Deposited on Fiberglass by CVD" 356 : 36-42, 2009

17 Aguero, F. N., "Catalytic Combustion of Volatile Organic Compounds in Binary Mixtures over MnOx/Al2O3 Catalyst" 91 : 108-112, 2009

18 Everaert, K, "Catalytic Combustion of Volatile Organic Compounds" B109 : 113-139, 2004

19 Tidahy, H. L., "Catalytic Activity of Copper and Palladium Based Catalysts for Toluene Total Oxidation" 119 : 317-320, 2007

20 Takaki, K., "Atmospheric Pressure of Nitrogen Plasmas in a Ferro-electric Packed Bed Barrier Discharge Reactor Part I: Modeling" 11 : 481-490, 2004

21 Chung-Liang Chang, "Applying spray pyrolysis to synthesize MnOx for decomposing isopropyl alcohol in ozone- and thermal-catalytic oxidation" 한국화학공학회 26 (26): 1047-1052, 2009

22 Besov, A. S., "Acceleration of Acetone Destruction Process Under Synergistic Action of Photocatalytic Oxidation and Barrier Discharge" 27 : 624-634, 2007

23 Tsuru, T., "A Photocatalytic Membrane Reactor for VOC Decomposition Using Pt-modified Titanium Oxide Porous Membranes" 280 : 156-162, 2006