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Continuous CO2 capture and reduction in one process: CO2 methanation over unpromoted and promoted Ni/ZrO2
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2018-03-21 , DOI: 10.1016/j.jcou.2018.03.013
Lingjun Hu , Atsushi Urakawa

The recently demonstrated concept to combine CO2 capture and utilization in one process using isothermal unsteady-state operation, namely CO2 capture and reduction (CCR), was applied for CO2 methanation using unpromoted and K- or La-promoted Ni/ZrO2 catalysts. Both K and La promoters significantly improve CO2 capture capacity and also the selectivity of CO2 conversion to methane. The K-promoted catalyst (Ni-K/ZrO2) captures a larger amount of CO2 at high temperature but the capture capacity drops at low temperature due to incomplete catalyst regeneration during the cyclic unsteady-state reaction condition. In contrast, the La-promoted catalyst (Ni-La/ZrO2) shows temperature-independent CO2 capture capacity and rapid reduction of captured CO2, thus leading to stable CCR performance. The nature of the active sites and mechanistic details were gained by TPR, reductive CO2-TPD and space- and time-resolved operando DRIFTS, holistically elucidating the effects of the promoters and their impacts on CCR activity.



中文翻译:

连续CO 2捕获和减少在一个过程:CO 2的甲烷化在未促进的,促进镍/的ZrO 2

最近展示的将等温非稳态操作在一个过程中结合CO 2捕集和利用的概念,即CO 2捕集和还原(CCR),被应用在使用未促进的和K或La促进的Ni / ZrO 2的CO 2甲烷化中催化剂。K和La促进剂都显着提高了CO 2的捕集能力,也提高了CO 2转化为甲烷的选择性。K促进的催化剂(Ni-K / ZrO 2)捕获大量的CO 2在高温下,但由于在循环非稳态反应条件下催化剂再生不完全,因此在低温下,捕集能力下降。相反,La促进的催化剂(Ni-La / ZrO 2)显示出与温度无关的CO 2捕集能力,并且捕集的CO 2迅速还原,因此导致了稳定的CCR性能。活性位点和机制细节的性质是由TPR上涨,还原CO 2 -TPD和空间和时间分辨operando漂移整体上阐明发起人及其对CCR活动的冲击效应。

更新日期:2018-03-21
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