类水滑石基镍系催化剂上的乙醇水蒸气重整反应分析-analysis of ethanol steam reforming reaction on hydrotalcite-like nickel catalyst.docxVIP

ABSTRACTSyngas (H2 + CO) is a key intermediate in the chemical industry for the production of a wide range of valuable fuels and chemicals such as clean synthetic gasoline, methanol, NH3 and H2. Ethanol steam reforming (ESR) is currently being considered as one of the best sustainable and economical alternative to fossil fuel-based processes for syngas and H2 production. However, the severe environment of high temperature and the co-existence of ethanol and high partial pressure of steam in ESR process create a significant challenge for the design of an effective Ni-based catalyst. On the other hand, most of the investigations of ESR focused on the development of the catalysts, only a few ones concerned the kinetics and mechanism of this reaction. Thus, this thesis is motivated firstly to prepare a novel and efficient core-shell Ni catalyst derived from hydrotalcite (HT)-like precursor. Secondly, effort is devoted to the kinetic study of ESR over a Ni/Mg-Al catalyst and the investigation of the effect of Ni loading on the intrinsic activity of this reaction.In chapter 2, a shell-core Ni@Mg-Al catalyst has been prepared via the reconstruction of a HT-derived Mg-Al mixed oxide in a Ni2+ nitrate solution. Results show that a part of Ni2+ can incorporate into the layered structure of the reconstructed hydrotalcite-like compound, but the others may be adsorbed and/or blocked by the forming flake-like sheets. At 700 oC, the H2 yield over one mole of Ni atoms demonstrates that the shell-core catalysts with much lower Ni contents perform better reactivities than that of the bulk 15 wt.% Ni/Mg-Al sample. The effects of temperature and space-time on the product distribution over the best Ni@Mg-Al catalyst indicate that methane steam and dry reforming as well as WGS are the key reactions during ESR under the conditions investigated. Moreover, the activity evaluations perfomed at 700 oC and very low space-time confirm the existence of C2H4 during the reforming process.In chapte