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协同促进 Ni-CaO 复合催化剂的 CO 捕集与原位转化。

Synergistic promotions between CO capture and in-situ conversion on Ni-CaO composite catalyst.

机构信息

Key Laboratory for Advanced Materials and Joint International Research Laboratory for Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.

出版信息

Nat Commun. 2023 Feb 22;14(1):996. doi: 10.1038/s41467-023-36646-2.

Abstract

The integrated CO capture and conversion (iCCC) technology has been booming as a promising cost-effective approach for Carbon Neutrality. However, the lack of the long-sought molecular consensus about the synergistic effect between the adsorption and in-situ catalytic reaction hinders its development. Herein, we illustrate the synergistic promotions between CO capture and in-situ conversion through constructing the consecutive high-temperature Calcium-looping and dry reforming of methane processes. With systematic experimental measurements and density functional theory calculations, we reveal that the pathways of the reduction of carbonate and the dehydrogenation of CH can be interactively facilitated by the participation of the intermediates produced in each process on the supported Ni-CaO composite catalyst. Specifically, the adsorptive/catalytic interface, which is controlled by balancing the loading density and size of Ni nanoparticles on porous CaO, plays an essential role in the ultra-high CO and CH conversions of 96.5% and 96.0% at 650 °C, respectively.

摘要

集成 CO 捕获与转化(iCCC)技术作为一种有前途的经济有效的碳中和方法正在蓬勃发展。然而,长期以来一直缺乏对吸附和原位催化反应之间协同效应的分子共识,这阻碍了其发展。在此,我们通过构建连续的高温钙循环和甲烷干重整过程来阐明 CO 捕获和原位转化之间的协同促进作用。通过系统的实验测量和密度泛函理论计算,我们揭示了在负载型 Ni-CaO 复合催化剂上,每个过程中产生的中间体的参与可以相互促进碳酸盐的还原途径和 CH 的脱氢途径。具体而言,通过平衡 Ni 纳米粒子在多孔 CaO 上的负载密度和尺寸来控制的吸附/催化界面,在 650°C 时分别以 96.5%和 96.0%的超高 CO 和 CH 转化率发挥了重要作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/98d4/9947161/adb463fabf54/41467_2023_36646_Fig1_HTML.jpg

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