Miaomiao Zhang, Yibo Gao, Wenlong Wang, Zhanlong Song, Yanpeng Mao
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Compared to Mg, Ca, and La promoters, Ni-Ce/AC catalyst was demonstrated the optimum catalyst for MW-DRM process, which showed the most excellent stability with good reforming activity over 96 % and 98 % for CH<sub>4</sub> and CO<sub>2</sub> conversion rates, respectively. By converting MW energy attenuation into heat and plasma, the locally-formed high-energy active sites composed of adjacent Ni, CeO<sub>2</sub> and AC support of the Ni-Ce/AC catalyst could contribute to achieving the effective and localized activation of CH<sub>4</sub> and CO<sub>2</sub> molecules, thus leading to the enhancement of the reforming activity and the reduction of the loss of AC support due to CO<sub>2</sub> gasification. Moreover, MW heating method could avoid the excessive consumption of the AC support in Ni-Ce/AC by increasing the graphitization degree of AC, thus prolonging the lifetime of the AC-based catalysts. 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引用次数: 0
摘要
微波增强甲烷干重整技术(MW-DRM)是一项极具吸引力的二氧化碳增值技术。然而,由于严重的碳沉积/损失或活性金属烧结,该工艺与碳基催化剂结合可能会遭受快速失活。研究了不同促进剂(Mg、Ca、La、Ce)改性的活性炭负载Ni催化剂在MW-DRM工艺中的应用。实验结果表明,在MW-DRM和常规加热DRM (CH-DRM)工艺中,由于交流载体的碳气化严重,活性金属的烧结严重,ca促进催化剂的重整活性和稳定性最差。与Mg、Ca和La助剂相比,Ni-Ce/AC催化剂表现出最优的稳定性,对CH4和CO2的转化率分别达到96% %和98% %,表现出良好的重整活性。通过将MW能量衰减转化为热量和等离子体,Ni- ce /AC催化剂局部形成的由相邻Ni、CeO2和AC载体组成的高能活性位点有助于实现CH4和CO2分子的有效和局部活化,从而提高重整活性,减少CO2气化导致的AC载体损失。同时,MW加热法通过提高AC的石墨化程度,避免了Ni-Ce/AC中AC载体的过度消耗,从而延长了AC基催化剂的使用寿命。总之,这些发现为MW与ac基催化剂在合成气生产中的协同作用提供了新的见解。
Effect of promoters on the syngas production in the microwave-enhanced methane dry reforming over Ni-x/AC (x = Mg, Ca, La, Ce) catalysts
Capitalizing on the targeted energy transfer, microwave-enhanced dry reforming of methane (MW-DRM) is an attractive CO2 valorization technology. However, this process coupled with carbon-based catalysts may suffer from rapid deactivation due to severe carbon deposition/loss or active metal sintering. In this study, activated carbon (AC)-supported Ni catalysts modified with different promoters (Mg, Ca, La, Ce) were investigated for MW-DRM process. As proved by the experiment results, Ca-promoted catalyst exhibited the worst reforming activity and stability in the MW-DRM and conventional heating DRM (CH-DRM) processes due to the severe carbon gasification of AC support and the severe sintering of the active metal. Compared to Mg, Ca, and La promoters, Ni-Ce/AC catalyst was demonstrated the optimum catalyst for MW-DRM process, which showed the most excellent stability with good reforming activity over 96 % and 98 % for CH4 and CO2 conversion rates, respectively. By converting MW energy attenuation into heat and plasma, the locally-formed high-energy active sites composed of adjacent Ni, CeO2 and AC support of the Ni-Ce/AC catalyst could contribute to achieving the effective and localized activation of CH4 and CO2 molecules, thus leading to the enhancement of the reforming activity and the reduction of the loss of AC support due to CO2 gasification. Moreover, MW heating method could avoid the excessive consumption of the AC support in Ni-Ce/AC by increasing the graphitization degree of AC, thus prolonging the lifetime of the AC-based catalysts. Above all, these findings provide new insights for the synergistic effect of MW with AC-based catalysts for syngas production.
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.