Abstract
Expanded multilayered vermiculite (VMT) was successfully used as catalyst support and Ni/VMT synthesized by microwave irradiation assisted synthesis (MIAS) exhibited excellent performance in our previous work. We also developed a two-dimensional porous SiO2 nanomesh (2D VMT-SiO2) by mixed-acid etching of VMT. Compared with three-dimensional (3D) MCM-41, 2D VMT-SiO2 as a catalyst support provided a superior position for implantation of NiO species and the as-obtained catalyst exhibited excellent performance. In this paper, we successfully synthesized a layered double hydroxide (LDH) using the spent liquor after mixed-acid etching of VMT, which mainly contained Mg2+ and Al3+. The as-calcined layered double oxide (LDO) was used as a catalyst support for CO methanation. Compared with Ni/MgAl-LDO, Ni/VMT-LDO had smaller active component particles; therefore, in this study, it exhibited excellent catalytic performance over the whole temperature range of 250–500 °C. Ni/VMT-LDO achieved the best activity with 87.88% CO conversion, 89.97% CH4 selectivity, and 12.47 × 10−2·s−1 turn over frequency (TOF) at 400 °C under a gas hourly space velocity of 20,000 mL/g/h. This study demonstrated that VMT-LDO as a catalyst support provided an efficient way to develop high-performance catalysts for synthetic natural gas (SNG) from syngas.
Highlights
Since carbon oxide methanation was discovered by Sabatier and Senderens in 1902, it has been well developed and widely used due to its capability as a chemical storage for excess H2 generated from renewable energy and a solution for greenhouse gas recycling [1,2,3]
MgAl-layered double hydroxide (LDH) has been used as a catalyst support in oxidation reactions [19,20], and the as-calcined samples, named layered double oxide (LDO) or mixed metal oxides (MMO) are used as supports due to their large specific surface area and the strong interaction between active components and the support [16]
Ni/VMT-LDO had smaller Ni nanoparticles compared with catalyst Ni/MgAl-LDO, which was ascribed to Fe and Ca modification improved the dispersion of nickel, which resulted in a low temperature activity
Summary
Since carbon oxide methanation was discovered by Sabatier and Senderens in 1902, it has been well developed and widely used due to its capability as a chemical storage for excess H2 generated from renewable energy and a solution for greenhouse gas recycling [1,2,3]. MgAl-LDH has been used as a catalyst support in oxidation reactions [19,20], and the as-calcined samples, named layered double oxide (LDO) or mixed metal oxides (MMO) are used as supports due to their large specific surface area and the strong interaction between active components and the support [16]. Li et al [21] found that the NiMgAl-LDO catalyst showed excellent CO methanation performance in high-temperature region: 400–650 ◦ C, the transmission electron microscopy (TEM) and X-ray diffraction (XRD) results indicated that upon calcination of the NiMgAl-LDH precursor, the NiO phase gains a strong interaction with.
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