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Oxy-CO2 reforming of CH4 on Ni-based catalysts: Evaluation of cerium and aluminum addition on the structure and properties of the reduced materials
Catalysis Today ( IF 5.3 ) Pub Date : 2020-09-10 , DOI: 10.1016/j.cattod.2020.09.004
Breno C. da Silva , Pedro Henrique C. Bastos , Roberto B.S. Junior , N.R. Checca , Denilson S. Costa , Roger Fréty , Soraia T. Brandão

Perovskites with the structural formula La1-xCexNi1-yAlyO3 (x = 0 y = 0; x = 0.05 y = 0; x = 0.05 y = 0.2 and x = 0.05 y = 0.5) were studied in the dry methane reforming in presence of oxygen or Oxy-Dry (OD). The materials were synthetized by the amorphous citrate method and characterized by XRD, in situ XRD under hydrogen and reactional (OD) atmospheres, TPR-H2, XRF, TPSR-OD, TPSR−CH4, TEM, HRTEM and TPO techniques. The catalytic performance was evaluated during 16 h of reaction, with a [CH4/CO2/O2] ratio = 4:2:1, at 800 °C and spatial velocity of 210.000 NL.h−1.kgcat−1. The addition of aluminum and cerium promoted an increase in the catalyst resistance to carbon poisoning, however, the higher the aluminum content was, the lower the reducibility of the perovskites and the nickel particle size. The La0.95Ce0.05Ni0.5Al0.5O3 sample showed the best results, with a maximum CH4 and CO2 conversion of 85 % and 86 % respectively and the higher syngas yield (45 % for CO and 48 % for H2). This sample presented the lowest Ni° particle size and carbon deposition after 16 h time on stream. No sign of deactivation was found for all the studied catalysts, showing the superior properties of catalysts prepared through perovskite-like mixed oxides.



中文翻译:

镍基催化剂上 CH4 的 Oxy-CO2 重整:铈和铝添加对还原材料结构和性能的评价

研究了具有结构式 La 1-x Ce x Ni 1-y Al y O 3 (x = 0 y = 0;x = 0.05 y = 0;x = 0.05 y = 0.2 和 x = 0.05 y = 0.5) 的钙钛矿在氧气或 Oxy-Dry (OD) 存在下的干甲烷重整中。材料通过无定形柠檬酸盐法合成,并通过XRD、氢气和反应(OD) 气氛下的原位XRD、TPR-H 2、XRF、TPSR-OD、TPSR-CH 4、TEM、HRTEM 和TPO 技术进行表征。在 16 小时的反应中评估催化性能,[CH 4 /CO 2 /O 2 ] 比 = 4:2:1,在 800 °C 和 210.000 NL.h -1 的空间速度.kg-1。铝和铈的加入促进了催化剂抗碳中毒能力的提高,但铝含量越高,钙钛矿的还原性和镍粒径越低。La 0.95 Ce 0.05 Ni 0.5 Al 0.5 O 3样品显示出最好的结果,最大 CH 4和 CO 2转化率分别为 85 % 和 86 %,合成气产率更高(CO 为 45 %,H 2为 48 %)。该样品在运行 16 小时后表现出最低的 Ni° 粒径和碳沉积。所有研究的催化剂均未发现失活迹象,表明通过类钙钛矿混合氧化物制备的催化剂具有优异的性能。

更新日期:2020-09-10
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