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충전층 플라즈마 반응기에서 Ni-CeO₂ / γ-Al₂O₃ 촉매를 이용한 프로페인-합성 가스 건식 개질
라미아 술타나(Lamia Sultana),Md. 샤히누르 라만(Md. Shahinur Rahman),M.S.P. 수드하카란(M.S.P. Sudhakaran),Md. 목터 호세인(Md. Mokter Hossain),목영선(Young Sun Mok) 한국청정기술학회 2019 청정기술 Vol.25 No.1
프로페인(C₃H8)의 건식 개질(CO₂ 개질)을 통한 합성 가스(H₂와 CO 혼합물) 제조를 위해 Ni-CeO₂/γ-Al₂O₃ 촉매가 충진된 유전체 장벽 방전 플라즈마 반응기를 사용하였다. 열 또는 플라즈마에 의해 환원된 Ni-CeO₂/γ-Al₂O₃ 촉매를 사용하여 C₃H8/CO₂ 비율 1/3, 총 유량 300 mL min<SUP>-1</SUP>에서 플라즈마-촉매 건식 개질을 수행하였다. 건식 개질에 대한 촉매 활성은 온도범위 500 ~ 600 ℃에서 평가되었다. Ni-CeO₂/γ-Al₂O₃ 촉매 제조를 위해 전구물질 수용액(질산니켈, 질산세륨)으로 함침된 γ-Al₂O₃를 공기 분위기에서 소성시킨 후, H₂/Ar 분위기에서 환원시켰다. 촉매 특성 조사에는 X-선 회절분석기(XRD), 투과 전자현미경(TEM), 전계 방출 주사전자현미경(FE-SEM), 승온 탈착(H₂-TPD, CO₂-TPD) 및 라만 분광기가 이용되었다. 열로 환원된 촉매와 비교하면 플라즈마 방전하에서 환원된 Ni-CeO₂/γ-Al₂O₃ 촉매가 개질 반응을 통한 합성 가스 생산에서 보다 우수한 촉매 활성을 나타내었다. 또한, 플라즈마로 환원된 Ni-CeO₂/γ-Al₂O₃가 개질 반응의 문제점인 탄소퇴적 관점에서 장기 촉매 안정성을 보여주었다. A dielectric barrier discharge (DBD) plasma reactor packed with Ni-CeO₂/γ-Al₂O₃ catalyst was used for the dry (CO₂) reforming of propane (DRP) to improve the production of syngas (a mixture of H₂ and CO) and the catalyst stability. The plasma-catalytic DRP was carried out with either thermally or plasma-reduced Ni-CeO₂/γ-Al₂O₃ catalyst at a C₃H8/CO₂ ratio of 1/3 and a total feed gas flow rate of 300 mL min<SUP>-1</SUP>. The catalytic activities associated with the DRP were evaluated in the range of 500 ~ 600 ℃. Following the calcination in ambient air, the γ-Al₂O₃ impregnated with the precursor solution (Ni(NO₃)₂ and Ce(NO₃)₂) was subjected to reduction in an H2/Ar atmosphere to prepare Ni-CeO₂/γ-Al₂O₃ catalyst. The characteristics of the catalysts were examined using X-ray diffraction (XRD), transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectrometry (EDS), temperature programmed reduction (H₂-TPR), temperature programmed desorption (H₂-TPD, CO₂-TPD), temperature programmed oxidation (TPO), and Raman spectroscopy. The investigation revealed that the plasma-reduced Ni-CeO₂/γ-Al₂O₃ catalyst exhibited superior catalytic activity for the production of syngas, compared to the thermally reduced catalyst. Besides, the plasma-reduced Ni-CeO₂/γ-Al₂O₃ catalyst was found to show long-term catalytic stability with respect to coke resistance that is main concern regarding the DRP process.
Muhammad Waqar Ahmed,Md. Shahinur Rahman,최수석,Ulugbek Shaislamov,양종근,Rai Suresh,이헌주 한국진공학회 2017 Applied Science and Convergence Technology Vol.26 No.5
The scope of this work is to determine and compare the effect of electron temperature (Te) and number density (Ne) on the yield rate and concentration of reactive chemical species (•OH, H2O2 and O3) in an argon, air and oxygen injected negative DC (0-4 kV) capillary discharge with water flow(0.1 L/min). The discharge was created between tungsten pin-to pin electrodes (Φ = 0.5 mm) separated by a variable distance (1-2 mm) in a quartz capillary tube (2 mm inner diameter, 4 mm outer diameter), with various gas injection rates (100-800 sccm). Optical emission spectroscopy (OES) of the hydrogen Balmer lines was carried out to investigate the line shapes and intensities as functions of the discharge parameters such as the type of gas, gas injection rate and inter electrode gap distances. The intensity ratio method was used to calculate Te and Stark broadening of Balmer β lines was adopted to determine Ne. The effects of Te and Ne on the reactive chemical species formation were evaluated and presented. The enhancement in yield rate of reactive chemical species was revealed at the higher electron temperature, higher gas injection rates, higher discharge power and larger inter-electrode gap. The discharge with oxygen injection was the most effective one for increasing the reactive chemical species concentration. The formation of reactive chemical species was shown more directly related to Te than Ne in a flowing water gas injected negative DC capillary discharge.
Ahmed, Muhammad Waqar,Rahman, Md. Shahinur,Choi, Sooseok,Shaislamov, Ulugbek,Yang, Jong-Keun,Suresh, Rai,Lee, Heon-Ju The Korean Vacuum Society 2017 Applied Science and Convergence Technology Vol.26 No.5
The scope of this work is to determine and compare the effect of electron temperature ($T_e$) and number density ($N_e$) on the yield rate and concentration of reactive chemical species ($^{\bullet}OH$, $H_2O_2$ and $O_3$) in an argon, air and oxygen injected negative DC (0-4 kV) capillary discharge with water flow(0.1 L/min). The discharge was created between tungsten pin-to pin electrodes (${\Phi}=0.5mm$) separated by a variable distance (1-2 mm) in a quartz capillary tube (2 mm inner diameter, 4 mm outer diameter), with various gas injection rates (100-800 sccm). Optical emission spectroscopy (OES) of the hydrogen Balmer lines was carried out to investigate the line shapes and intensities as functions of the discharge parameters such as the type of gas, gas injection rate and inter electrode gap distances. The intensity ratio method was used to calculate $T_e$ and Stark broadening of Balmer ${\beta}$ lines was adopted to determine $N_e$. The effects of $T_e$ and $N_e$ on the reactive chemical species formation were evaluated and presented. The enhancement in yield rate of reactive chemical species was revealed at the higher electron temperature, higher gas injection rates, higher discharge power and larger inter-electrode gap. The discharge with oxygen injection was the most effective one for increasing the reactive chemical species concentration. The formation of reactive chemical species was shown more directly related to $T_e$ than $N_e$ in a flowing water gas injected negative DC capillary discharge.