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沉积沉淀法制备的Ni/γ-Al₂O₃上的CO和CO₂甲烷化反应

CO and CO₂ Methanation Over Ni/γ-Al₂O₃ Prepared by Deposition-Precipitation Method.

作者信息

Le Thien An, Kang Jong Kyu, Lee Sae Ha, Park Eun Duck

机构信息

Department of Chemical Engineering and Department of Energy Systems Research, Ajou University, 206 Worldcup-ro, Yeongtong-gu, Suwon 16499, Republic of Korea.

出版信息

J Nanosci Nanotechnol. 2019 Jun 1;19(6):3252-3262. doi: 10.1166/jnn.2019.16585.

Abstract

Various Ni catalysts supported on γ-Al₂O₃ were prepared by a wet impregnation (WI) method and deposition-precipitation (DP) method with different precipitants and applied to CO and CO₂ methanation. The prepared catalysts were characterized by various techniques including nitrogen physisorption, X-ray diffraction (XRD), temperature-programmed reduction with H₂ (H₂-TPR), H₂ chemisorption, transmission electron microscopy (TEM), thermogravimetric analysis (TGA), and inductively coupled plasma-atomic emission spectroscopy (ICP-AES). Irrespective of kinds of precipitant, the Ni/γ-Al₂O₃ catalysts prepared with a DP method showed a remarkable enhanced catalytic performance in CO and CO₂ methanation compared with the Ni/γ-Al₂O₃ catalyst prepared with a WI method owing to the higher catalytic active surface area (CASA). In the case of Ni/γ-Al₂O₃ catalysts prepared with a DP method, the high calcination temperatures are not favorable for the high catalytic activity due to the decreased reduction degree of Ni oxide species and CASA. The reduction degree of Ni oxide species can be increased with reduction temperature. However, the higher reduction temperature above 500 °C is not desirable to achieve the high catalytic activity because of the decreased CASA. The selective CO methanation was also accomplished at lower temperatures over the Ni/γ-Al₂O₃ catalyst prepared with a DP method than over the Ni/γ-Al₂O₃ catalyst prepared with a WI method.

摘要

通过湿浸渍(WI)法和沉积沉淀(DP)法,使用不同沉淀剂制备了负载在γ -Al₂O₃上的各种镍催化剂,并将其应用于CO和CO₂甲烷化反应。采用多种技术对制备的催化剂进行了表征,包括氮气物理吸附、X射线衍射(XRD)、氢气程序升温还原(H₂-TPR)、H₂化学吸附、透射电子显微镜(TEM)、热重分析(TGA)以及电感耦合等离子体原子发射光谱(ICP-AES)。无论沉淀剂种类如何,与通过WI法制备的Ni/γ -Al₂O₃催化剂相比,采用DP法制备的Ni/γ -Al₂O₃催化剂在CO和CO₂甲烷化反应中表现出显著增强的催化性能,这归因于更高的催化活性表面积(CASA)。对于采用DP法制备的Ni/γ -Al₂O₃催化剂,由于Ni氧化物物种的还原度和CASA降低,高温煅烧不利于高催化活性。Ni氧化物物种的还原度可随还原温度升高而增加。然而,由于CASA降低,高于500℃的较高还原温度不利于实现高催化活性。与通过WI法制备的Ni/γ -Al₂O₃催化剂相比,采用DP法制备的Ni/γ -Al₂O₃催化剂在较低温度下也能实现选择性CO甲烷化。

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