CO2 dry reforming of CH4 with Sr and Ni co-doped LaCrO3 perovskite catalysts

CO2 dry reforming of CH4 with Sr and Ni co-doped LaCrO3 perovskite catalysts
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Sr、Ni共掺杂LaCrO3钙钛矿催化剂CO2干重整CH4

DOI:
10.1016/j.apsusc.2019.144699
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发表时间:
2020-03
影响因子:
6.7
通讯作者:
Jian Li
Jian Li
中科院分区:
材料科学1区
文献类型:
--
作者:
Tong Wei;Lichao Jia;Jing-Li Luo;Bo Chi;Jian Pu;Jian Li

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制备催化剂La0.8−xSrxCr0.85Ni0.15O3(x = 0、0.1、0.2和0.3; P-80、P-71、P-62和P-53),并在H2中还原(R-80、R-71、R-62和R-53)用于甲烷的CO2-干重整(CO2-DRM)。P-80、P-71和P-62是单相钙钛矿; P-53含有额外的NiO和SrCrO 4。Ni颗粒在R-80、R-71和R-62中以强烈的界面相互作用出溶,而在R-53中则由NiO还原产生。增加Sr浓度增加载体的碱度和氧空位浓度。R-53在低于650 °C时表现出最高的CH 4和CO2转化率,在高于650 °C时由于碳沉积而降低到最低,而R-62表现出最高的性能,在800 °C时CH 4和CO2转化率为90%,这是由于强的出溶Ni颗粒/载体界面相互作用以及载体的高碱度和氧空位浓度。在750 °C和0.3 × 104 ml g−1h−1下,R-62的性能稳定,甲烷和二氧化碳的转化率接近90%,H2和CO的选择性大于95%。
Catalysts La0.8−xSrxCr0.85Ni0.15O3(x = 0, 0.1, 0.2 and 0.3; P-80, P-71, P-62 and P-53) are prepared and reduced (R-80, R-71, R-62 and R-53) in H2for CO2-dry reforming of methane (CO2-DRM). P-80, P-71 and P-62 are single-phase perovskite; P-53 contains additional NiO and SrCrO4. Ni particles are exsolved in R-80, R-71 and R-62 with a strong interfacial interaction; whereas those in R-53 are produced by NiO reduction. Increasing Sr concentration increases basicity and oxygen vacancy concentration of the support. R-53 demonstrates the highest conversion of CH4and CO2below 650 °C, which decreases to the lowest above 650 °C due to carbon deposition, while R-62 shows the highest performance with CH4and CO2conversions on the level of 90% at 800 °C because of the strong exsolved Ni particle/support interfacial interaction and the high basicity and oxygen vacancy concentration of the support. The performance of R-62 increases with the decrease of gas hourly space velocity (GHSV) from 1.2 to 0.3 × 104ml g−1h−1, and remains stable at 750 °C and 0.3 × 104ml g−1h−1with conversions of CH4and CO2near 90% and selectivities of H2and CO above 95%.
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