Precious Metal Doped Ni–Mg/Ceria–Zirconia Catalysts for Methane Conversion to Syngas by Low Temperature Bi-reforming
Precious Metal Doped Ni–Mg/Ceria–Zirconia Catalysts for Methane Conversion to Syngas by Low Temperature Bi-reforming
复制标题
贵金属掺杂 Ni-Mg/Ceria-Zirconia 催化剂用于低温双重整将甲烷转化为合成气
DOI：
10.1007/s10562-018-2310-y
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发表时间：
2018
影响因子：
2.8
通讯作者：
J. Kuhn
中科院分区：
文献类型：
--
作者：
N. Elsayed;D. Maiti;B. Joseph;J. Kuhn
摘要研究了低温（450-600°C）甲烷在铂（0.16 wt%）或钯（0.13 wt%）、镍（1.4 wt%）和镁（1.0 wt%）固定在氧化铈载体（0.16 pt和0.13 pd）上的双重整反应。采用进料比为3:1:2的CH4:CO2:H2O的双重整研究表明，对于0.16Pt催化剂，在500 ~ 600°C之间，H2:CO比接近所需的2，与传统条件下的双重整相一致。与干重整或蒸汽重整以及其他CH4:CO2:H2O比相比，这种H2:CO比是理想的（接近2）。反应研究表明，在500°C时，ch4转化率随GHSV （68,000-272,000 h−1）的增加而降低，在GHSV为136,000 h−1时，ch4转化率随温度的增加而增加。然而，与钯基催化剂（H2:CO比为1.6-3.0）相比，pt基催化剂的H2:CO比在1.9 - 2.2（温度≥500°C）之间更为一致，这与rWGS活性的提高和更强的co2吸附有关。该研究表明，尽管在这种低温条件下运行，仍可以实现合理的ch4转化率和接近2的H2:CO比，并可能使甲烷转化为增值产品的过程加强。图形抽象
AbstractLow temperature (450–600 °C) bi-reforming of methane was studied over platinum (0.16 wt%) or palladium (0.13 wt%) along with nickel (1.4 wt%) and magnesium (1.0 wt%) immobilized onto a ceria–zirconia support (termed 0.16Pt and 0.13Pd). Bi-reforming studies using a feed ratio of 3:1:2 for CH4:CO2:H2O, respectively, showed that the H2:CO ratio neared the desired ratio of 2 between 500 and 600 °C for the 0.16Pt catalyst and consistent with bi-reforming at more traditional conditions. This H2:CO ratio was desirable (near 2) compared to dry or steam reforming alone, as well as to other CH4:CO2:H2O ratios. Reaction studies showed that CH4conversion decreased with increasing GHSV (68,000–272,000 h−1) at 500 °C and increased with increasing temperature at a GHSV of 136,000 h−1for both catalyst systems. However, the Pt-based catalyst had more consistent H2:CO ratios between 1.9 and 2.2 (T ≥ 500 °C) compared to its Pd counterpart (H2:CO ratios of 1.6–3.0), which was linked to the increased rWGS activity and stronger CO2adsorption. This study indicates reasonable CH4conversions and H2:CO ratio near 2 can be achieved despite operating in this low temperature regime and may enable intensified processes for the conversion of methane to value-added products.Graphical Abstract