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Enhanced H2-Rich Gas Production via Steam Reforming of Toluene over Ni-Based Hydrotalcite-Derived Catalysts at Low Temperature
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-06-07 , DOI: 10.1021/acssuschemeng.1c03122 Jie Ren 1 , Fei-Long Yang 2 , Yi-Ling Liu 2
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-06-07 , DOI: 10.1021/acssuschemeng.1c03122 Jie Ren 1 , Fei-Long Yang 2 , Yi-Ling Liu 2
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Tar reforming in the presence of Ni-based catalysts is a promising method for syngas production during biomass gasification, but common Ni-based catalysts (e.g., Ni/Al2O3) are easily deactivated during actual operation. In this work, Mg–Al hydrotalcite was synthesized by coprecipitation, followed by Ni impregnation and calcination, to obtain a Ni/MgAl catalyst, which exhibited excellent activity and stability for toluene (as a tar model compound) conversion. After various types of characterization and experimental investigations, the reaction and deactivation pathways were explained. The optimized Ni/MgAl-10 catalyst with better Ni dispersion, tailored basicity, and specific surface area showed remarkable toluene conversion (98.5%) and H2 production (609 mmol/g-Ni) at a low temperature. On the basis of calculations of the apparent activation energy and turnover frequency (TOF), Ni/MgAl-10, with the lowest activation energy (25.6 kJ/mol) and highest TOF value (4.31 h–1), was found to be the most active catalyst for H2-rich gas production. Moreover, the spent catalyst was systemically characterized by SEM and XPS, and mechanisms of reaction and deactivation were proposed. This work developed a strategy for the design of an active and stable catalyst for toluene reforming, which has potential for application in the reforming of real tar during biomass gasification.
中文翻译：
低温下在镍基水滑石衍生催化剂上通过甲苯蒸汽重整提高富H 2气体产量
在Ni基催化剂存在下的焦油重整是生物质气化过程中合成气生产的一种有前景的方法，但常见的Ni基催化剂（如Ni/Al 2 O 3）在实际操作中很容易失活。在这项工作中，Mg-Al 水滑石通过共沉淀合成，然后 Ni 浸渍和煅烧，以获得 Ni/MgAl 催化剂，该催化剂对甲苯（作为焦油模型化合物）的转化表现出优异的活性和稳定性。经过各种类型的表征和实验研究，解释了反应和失活途径。优化的 Ni/MgAl-10 催化剂具有更好的 Ni 分散性、定制的碱度和比表面积，表现出显着的甲苯转化率 (98.5%) 和 H 2在低温下产生 (609 mmol/g-Ni)。根据表观活化能和转换频率 (TOF) 的计算，发现活化能最低 (25.6 kJ/mol) 和最高 TOF 值 (4.31 h –1 ) 的Ni/MgAl-10是富H 2气体生产的最活性催化剂。此外，用SEM和XPS对废催化剂进行了系统表征，并提出了反应和失活的机理。这项工作为设计一种活性稳定的甲苯重整催化剂开发了一种策略，该催化剂在生物质气化过程中真正焦油的重整中具有应用潜力。
更新日期：2021-06-21
中文翻译：
低温下在镍基水滑石衍生催化剂上通过甲苯蒸汽重整提高富H 2气体产量
在Ni基催化剂存在下的焦油重整是生物质气化过程中合成气生产的一种有前景的方法，但常见的Ni基催化剂（如Ni/Al 2 O 3）在实际操作中很容易失活。在这项工作中，Mg-Al 水滑石通过共沉淀合成，然后 Ni 浸渍和煅烧，以获得 Ni/MgAl 催化剂，该催化剂对甲苯（作为焦油模型化合物）的转化表现出优异的活性和稳定性。经过各种类型的表征和实验研究，解释了反应和失活途径。优化的 Ni/MgAl-10 催化剂具有更好的 Ni 分散性、定制的碱度和比表面积，表现出显着的甲苯转化率 (98.5%) 和 H 2在低温下产生 (609 mmol/g-Ni)。根据表观活化能和转换频率 (TOF) 的计算，发现活化能最低 (25.6 kJ/mol) 和最高 TOF 值 (4.31 h –1 ) 的Ni/MgAl-10是富H 2气体生产的最活性催化剂。此外，用SEM和XPS对废催化剂进行了系统表征，并提出了反应和失活的机理。这项工作为设计一种活性稳定的甲苯重整催化剂开发了一种策略，该催化剂在生物质气化过程中真正焦油的重整中具有应用潜力。
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