SiO2气凝胶负载的Ni催化剂在甲烷部分氧化制合成气反应中的催化性能及稳定性

doi:10.3866/PKU.WHXB201308201

Abstract

Abstract:

Two types of aerogel silica, denoted as SiO₂-A(or B)G are synthesized with either solvent substitution (A) or solvent substitution-surface modification (B) under atmospheric conditions. Aerogel silicasupported Ni catalysts are then prepared via impregnated (IM) and polyvinylpyrrolidone (PVP)-added IM methods, and their performances for the partial oxidation of methane (POM) are investigated. The similar initial catalytic performances (activity and selectivity) are observed over the different Ni/SiO₂ catalysts. With respect to POMstability, Ni/SiO₂-BG is significantly worse than Ni/SiO₂-AG, while catalysts with PVP addition (during preparation) exhibit a significant improvement. In this case, Ni/SiO₂-BG-PVPis comparable to Ni/SiO₂-AG-PVP. We characterize the catalysts with X-ray diffraction (XRD), temperature-programmed hydrogen reduction (H₂-TPR), transmission electron microscopy (TEM), and Brunauer-Emmett-Teller (BET) analysis. We find that there are hydroxyls on the SiO₂-AG surface that favor their interaction with hydrophilic metal species, while on the SiO₂-BGsurface there are organic groups that do not interact with hydrophilic metal species. In addition, with the help of PVP, metal species can access the deep pores of hydrophilic/hydrophobic silica gels. Then, the contraction of the silica framework and the growth of metal particles are inhibited during calcinations, enhancing interactions between Ni and the silica gels. These (benefits fromsurface hydroxyls and PVP) result in significant improvements in the catalysts with respect to POMstability.

Key words: SiO₂, Aerogel, POM, Hydroxyl, PVP, Stability

LI Qi, HOU Yu-Hui, DONG Ling-Yu, HUANG Ming-Xiang, WENG Wei-Zheng, XIA Wen-Sheng, WAN Hui-Lin. Catalytic Behaviors and Stability of Aerogel Silica-Supported Ni Catalysts for the Partial Oxidation of Methane into Synthesis Gas[J]. Acta Phys. -Chim. Sin. 2013, 29(10), 2245-2254. doi: 10.3866/PKU.WHXB201308201

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Catalytic Behaviors and Stability of Aerogel Silica-Supported Ni Catalysts for the Partial Oxidation of Methane into Synthesis Gas

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