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CO2 methanation over nickel-based catalysts supported on MCM-41 with in situ doping of zirconium
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2020-09-07 , DOI: 10.1016/j.jcou.2020.101304
Meng Yang , Zhu Lingjun , Zhu Xiaonan , Reubroycharoen Prasert , Wang Shurong

CO2 methanation with H2 derived from renewable energy is an effective strategy to reduce the emission of CO2 by converting CO2 into a high-value fuel. Ni-based catalysts have been widely studied due to their low cost and relatively good catalytic performance. However, to reach high catalytic activity at low temperature and good stability at high temperature, the Ni-based catalysts should be improved. A special catalyst support was prepared by hydrothermal synthesis with in situ doping of Zr, namely, Zr(x)@MCM-41. A series of supported Ni-based catalysts, Ni/Zr(x)@MCM-41, was prepared by citric-acid-assisted impregnation. The structure and physicochemical properties of catalysts were characterized by BET, XRD, TEM, CO2-TPD and TG. The strengthened interaction between Zr and Ni favoured the spillover of H absorbed on Ni to the support, which promoted the hydrogenation of CO2 and intermediates COad on the support and increased the CO2 conversion at low temperature. Simultaneously, with the addition of Zr, the amount of strong basic sites decreased, and the amount of surface oxygen species increased, which not only inhibited the carbon deposition but also enabled the deposited carbon to be reoxidized and participate in the reaction, so the selectivity of CH4 slightly improved. However, excessive addition of Zr will reduce the reactivity of the catalysts, since the order of the pore structure decreases, and many irregular pore structures are generated. The catalyst Ni/@Zr(0.01)@MCM-41 with an appropriate Zr content reached a high CO2 conversion of 88.6 % and a CH4 selectivity of 96.5 % at 280 °C and 1 MPa.



中文翻译:

在原位掺杂锆的MCM-41上负载的镍基催化剂上进行CO 2甲烷化

用可再生能源中的H 2进行CO 2甲烷化是一种有效的策略,可通过将CO 2转化为高价值燃料来减少CO 2的排放。镍基催化剂由于其低成本和相对良好的催化性能而被广泛研究。然而,为了在低温下达到高催化活性和在高温下具有良好的稳定性,应该改进Ni基催化剂。通过水热合成和原位掺杂Zr制备了一种特殊的催化剂载体,即Zr(x)@ MCM-41。通过柠檬酸辅助浸渍制备了一系列负载型Ni基催化剂Ni / Zr(x)@ MCM-41。用BET,XRD,TEM,CO 2对催化剂的结构和理化性质进行了表征。-TPD和TG。Zr与Ni之间的相互作用增强,有利于Ni上吸附的H溢出到载体上,这促进了CO 2和中间体CO ad的氢化,并增加了低温下的CO 2转化率。同时,通过添加Zr,强碱性位点的数量减少,表面氧种类的数量增加,这不仅抑制了碳的沉积,而且使沉积的碳能够被再氧化并参与反应,因此具有选择性。 CH 4之略有改善。然而,过量添加Zr将降低催化剂的反应性,因为孔结构的顺序降低,并且产生许多不规则的孔结构。具有合适Zr含量的催化剂Ni / @ Zr(0.01)@ MCM-41在280℃和1MPa下达到88.6%的高CO 2转化率和96.5%的CH 4选择性。

更新日期:2020-09-08
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