Abstract The long-time stability test of Zn-Cr catalysts for isobutanol synthesis via syngas under vigorous reaction conditions was reported in this work, and the deactivation mechanism over these catalysts for isobutanol synthesis was discussed deeply. Based on the analysis of TEM, XRD, TG-DT, ICP and N2 adsorption-desorption isotherms, some traditional causes of deactivation, such as sintering, coke deposition, the formation of inactive species, and the loss of active metals, are negligible over the Zn-Cr catalyst. From the IR and XAS analysis, the spent catalyst presents a lower level of cation disorder distribution with fewer defects and oxygen vacancies on the surface, suggesting that the nanostructural change of the Zn-Cr catalyst will be the main cause of catalyst deactivation. The physico-chemical properties of the fresh and spent catalysts were investigated by XPS, CO2-TPD and NH3-TPD analyses, and the results show that the structural change would affect the oxygen state and the acidity-basicity over the surface of the catalysts. The loss of hydroxyl groups, as well as the weak synergistic effects between acidity and basicity over the spent catalyst surface, also plays a crucial role in the catalyst deactivation of the Zn-Cr catalyst.

中文翻译：

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合成气合成异丁醇Zn-Cr二元催化剂失活机理的深入研究

摘要 本文报道了合成气合成异丁醇Zn-Cr催化剂在剧烈反应条件下的长期稳定性试验，并对这些催化剂用于异丁醇合成的失活机理进行了深入探讨。基于对TEM、XRD、TG-DT、ICP和N2吸附-解吸等温线的分析，一些传统的失活原因，如烧结、焦炭沉积、非活性物种的形成和活性金属的损失，可以忽略不计。 Zn-Cr 催化剂。从IR和XAS分析来看，废催化剂的阳离子无序分布水平较低，表面缺陷和氧空位较少，表明Zn-Cr催化剂的纳米结构变化将是催化剂失活的主要原因。通过 XPS、CO2-TPD 和 NH3-TPD 分析研究了新催化剂和废催化剂的理化性质，结果表明结构变化会影响催化剂表面的氧状态和酸碱度。羟基的损失，以及酸碱度在废催化剂表面的弱协同作用，也在 Zn-Cr 催化剂的催化剂失活中起着至关重要的作用。