Browsing by Author "Tsai, Ping-Wen"

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Metal substituted pyrochlore phase LixLa2-xCe1.8Ru0.2O7- (x=0.0-0.6) as an effective catalyst for oxidative and auto-thermal steam reforming of ethanol
(2019-03-21)
Hsieh, Ho-Chen
;
Chang, Yuan-Chia
;
Tsai, Ping-Wen
;
Lin, Yen-Yu
;
Chuang, Yu-Chun
Pyrochlore phase LixLa2-xCe1.8Ru0.2O7- (x = 0.0-0.6) [LLCRO] substituted by Li and Ru in A and B sites was synthesized and studied for performance in oxidative steam and auto-thermal reforming of ethanol (OSRE, ATR). The samples were characterized by powder X-ray diffraction (PXRD), X-ray absorption spectroscopy (XAS), and X-ray photoelectron spectroscopy (XPS) to examine the effect of substituted Li+ and Run+ on OSRE performance. The results indicated that the substituted Li ions modified the oxidation states of Ru and Ce in LLCRO, which led to oxygen vacancies/mobility and played an important role in the catalytic performance of OSRE. Using LLCRO as the catalyst and supported by Al2O3, La2Zr2O7 (LZO) was investigated for its hydrogen production performance. The catalytic stability of the LLCRO (x = 0.6)/LZO catalysts was tested at 350 degrees C under oxidative steam conditions (OSRE) and showed a stable ethanol conversion and hydrogen production (X-EtOH = 98(3)%; S-H2 = 95(3)%). Under autothermal conditions (ATR), the LLCRO (x = 0.6) catalyst supported by LZO exhibited a stable catalytic performance with an average ethanol conversion and hydrogen selectivity of 90(3)% and 71(4)%, respectively. Carbon deposition was significantly suppressed during the OSRE and ATR processes on LLCRO (x = 0.6) catalysts supported by LZO, whereas, a significant carbon deposition was observed for LLCRO (x = 0.6)/Al2O3 as the catalyst. These results indicate that LLCRO (x = 0.6) supported by LZO is an effective catalyst for hydrogen production. The enhanced activity was attributed to the effectively suppressed carbon deposition and the sintering of highly dispersed Ru ions in the LLCRO catalyst, which may be due to the strong binding between the catalyst and LZO.
Oxidative steam reforming of ethanol over MxLa2-xCe1.8Ru0.2O7-delta (M = Mg, Ca) catalysts: effect of alkaline earth metal substitution and support on stability and activity
(2019-12-02)
Hsieh, Ho-Chen
;
Tsai, Ping-Wen
;
Chang, Yuan-Chia
;
Weng, Sheng-Feng
;
Sheu, Hwo-Shuenn
Alkaline earth metal substitutions on the A-site of pyrochlore oxide MxLa2-xCe1.8Ru0.2O7-delta (M = Mg, Ca) were studied as catalyst materials for oxidative/autothermal steam reforming of ethanol (OSRE/ATR). The as-prepared oxides were synthesized by a combustion method and characterized using powder X-ray diffraction (PXRD), and X-ray photoelectron and absorption spectroscopy (XPS and XAS). PXRD Rietveld analysis and elemental analysis (ICP-AES) support the formation of a pyrochlore-type structure (space group Fd3m) with a distorted coordination environment. The substitution of Mg²⁺ and Ca²⁺ ions affects the oxidation states of Ce^4+/3+ and Ruⁿ⁺ ions and creates oxygen vacancies, which leads to enhanced catalytic activity and reduced ethylene selectivity. A long-term stability test showed optimized catalysts Mg0.3La1.7Ce1.8Ru0.2O7-delta and Ca0.2La1.8Ce1.8Ru0.2O7-delta with SH2 = 101(1)% and SH2 = 91(2)% under OSRE conditions. The initial operation temperatures were lower than that of the unsubstituted catalyst La2Ce1.8Ru0.2O7-delta. Catalysts supported on La2Zr2O7 showed stable OSRE/ATR performance and low carbon deposition compared to catalysts supported on Al2O3. We ascribe the enhanced activity to well-dispersed alkaline earth metal and Ru ions in a solid solution structure, synergistic effects of (Mg, Ca)²⁺/Ce^3+/4+/Ruⁿ⁺ ions, and a strong catalyst-support interaction that optimized the ethanol conversion and hydrogen production.