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Investigating the dynamic structural changes on Cu/CeO2 catalysts observed during CO2 hydrogenation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2019-12-09 , DOI: 10.1016/j.jcat.2019.11.017
Pramod Sripada , Justin Kimpton , Anders Barlow , Tim Williams , Shalini Kandasamy , Sankar Bhattacharya

CO2 hydrogenation is one route for partial CO2 abatement while producing valuable chemical products. Cu/CeO2 catalysts have attracted great interest as materials that facilitate the efficient hydrogenation of CO2 into methanol and CO. This paper investigates the effect of preparation methods on the structure, function and activity of Cu/CeO2 catalysts. The catalysts have been prepared by deposition–precipitation (DP) and the co-precipitation (CP) methods. The activity tests for the catalysts were conducted in a high-pressure packed bed reactor in the temperature range of 200–300 °C at 50 bar pressure. The DP catalyst showed higher methanol productivity and lower methanol selectivity compared its CP counterpart. The reasons for the higher performance of the DP catalyst and other structural and functional differences have been investigated through in-depth characterization using synchrotron radiated in-situ powder diffraction, DRIFTS, XPS, HR-TEM, TPR and N2O decomposition used to determine copper surface area. The higher methanol productivity in the DP catalyst was attributed to the higher Cu surface area and dispersion. Additionally, the in-situ synchrotron-based powder diffraction measurements provide fundamental insights on the interesting differences in the CeO2 structure i.e. the lattice parameter and the lattice microstrain during the reduction step that could be attributed to the size difference in the CeO2 support nanoparticles.



中文翻译:

研究在CO 2加氢过程中观察到的Cu / CeO 2催化剂的动态结构变化

CO 2加氢是部分CO 2减排同时生产有价值的化学产品的一种途径。Cu / CeO 2催化剂作为促进CO 2有效加氢成甲醇和CO的材料引起了人们的极大兴趣。本文研究了制备方法对Cu / CeO 2的结构,功能和活性的影响。催化剂。催化剂是通过沉积沉淀(DP)和共沉淀(CP)方法制备的。催化剂的活性测试是在高压填充床反应器中,温度范围为200-300°C,压力为50 bar的条件下进行的。与CP催化剂相比,DP催化剂显示出更高的甲醇生产率和更低的甲醇选择性。通过使用同步辐射原位粉末衍射,DRIFTS,XPS,HR-TEM,TPR和N 2进行深入表征,研究了DP催化剂性能更高以及其他结构和功能差异的原因。O分解用于确定铜的表面积。DP催化剂中较高的甲醇生产率归因于较高的Cu表面积和分散度。此外,基于原位同步加速器的粉末衍射测量提供了有关CeO 2结构有趣差异的基本见解,即还原步骤期间的晶格参数和晶格微应变,这可能归因于CeO 2载体纳米粒子的尺寸差异。

更新日期:2019-12-09
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