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首页> 外文期刊>Catalysis science & technology >Mechanistic insights into the CO2 capture and reduction on K-promoted Cu/Al2O3 by spatiotemporal operando methodologies
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Mechanistic insights into the CO2 capture and reduction on K-promoted Cu/Al2O3 by spatiotemporal operando methodologies

机译:Mechanistic insights into the CO2 capture and reduction on K-promoted Cu/Al2O3 by spatiotemporal operando methodologies

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摘要

Integrated CO2 capture and conversion processes bring the promise of drastic abatement of CO2 emission together with its valorisation to chemical building blocks such as CH4 and CO. Isothermal CO2 capture and reduction (CCR) on a K-promoted Cu/Al2O3 was recognised as an effective catalytic strategy for removing CO2 from diluted stream and converting it to syngas (H2 + CO) employing green H2 as reducing agent. The dual functionality of the catalyst is the key of this dynamic process, in which the alkaline metal introduces the capture functionality and copper ensures the selective conversion of the captured CO2 to CO. However, the highly dynamic state of the catalyst at reaction conditions represents a barrier for the identification of the catalytic mechanism of CCR, which is vital for rational process improvement and design. In this work, we conducted a mechanistic investigation of CCR by means of spatiotemporal operando methodologies, gaining insights into dynamic variation of temperature, gas concentration and reactive surface species in the CCR reactor. The results show the unique potassium state exothermically captures CO2 as surface carbonates which can be reduced to CO rapidly under H2 atmosphere. When the surface carbonates are transformed to formates the reaction path is altered and the reduction to CO becomes slower. By designing controlled catalytic experiments, we further demonstrate the active involvement of CO in the capture mechanism and the effectiveness of CO2 capture in presence of an oxidised surface, extending the perspectives and suitability of CCR to treat actual complex effluent streams.
机译:集成的二氧化碳捕获和转化过程带来激烈的承诺减排二氧化碳排放连同其维持价格化学建筑材料如CH4和有限公司等温二氧化碳捕获和减少(CCR)K-promoted铜/氧化铝被认可为一个有效的催化去除二氧化碳的策略从稀释流并将它转化为合成气(H2 + CO)采用绿色氢气作为还原剂。的双功能催化剂是关键这个动态的过程中,碱性金属和介绍了捕获功能保证了铜选择性的转换捕获二氧化碳有限公司。然而,高度动态催化剂在反应条件的状态代表一个障碍的识别CCR的催化机制,这是至关重要的为rational过程改进和设计。这项工作,我们进行了机械CCR通过时空的调查operando方法、获得的见解动态变化的温度,气体浓度和表面活性物种CCR反应堆。钾状态exothermically捕捉二氧化碳表面碳酸盐可以简化为有限公司迅速在H2气氛。碳酸盐转化整合反应路径是改变和减少有限公司变得缓慢。实验中,我们进一步展示活动参与公司的捕获机制和存在的二氧化碳捕获的有效性一个表面氧化,延长视角和适用性的CCR治疗实际复杂废水流。

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