文献类型：期刊文献

英文题名：Potassium-Promoted Limestone for Preferential Direct Hydrogenation of Carbonates in Integrated CO2 Capture and Utilization

作者：Sun, Shuzhuang[1,2];Chen, Zheng[3];Xu, Yikai[2,4];Wang, Yuanyuan[2];Zhang, Yingrui[2];Dejoie, Catherine[5];Xu, Shaojun[6,7];Xu, Xin[3];Wu, Chunfei[2]

机构：[1]Zhengzhou Univ, Sch Chem Engn, Zhengzhou 450001, Peoples R China;[2]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT7 1NN, North Ireland;[3]Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China;[4]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China; East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]European Synchrotron Radiat Facil, F-38043 Grenoble, France;[6]Univ Manchester, Dept Chem Engn, Manchester M13 9PL, England;[7]UK Catalysis Hub, Res Complex Harwell, Didcot OX11 0FA, England

年份：2023

卷号：4

期号：1

起止页码：72

外文期刊名：JACS AU

收录：WOS:【ESCI(收录号:WOS:001146726100001)】；

基金：The authors gratefully acknowledge financial support from the China Scholarship Council (reference number:201906450023). This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sk & lstrok;odowska-Curie grant agreement No 823745. The UK Catalysis Hub is kindly thanked for the resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026939/1, EP/R026815/1, EP/R026645/1, EP/R027129/1, or EP/M013219/1(biocatalysis). Prof Sihai Yang is kindly thanked for the resources and support provided for the access to the beamline ID22 of European Synchrotron Research Facility (ESRF) at Grenoble, France.

语种：英文

外文关键词：carbon dioxide; hydrogenation; selectivity; integrated CO2 capture and utilization; transition-metalsfree catalysts; reverse water-gas shift reaction; dual functional material

摘要：Integrated CO2 capture and utilization (ICCU) via the reverse water-gas shift (RWGS) reaction offers a particularly promising route for converting diluted CO2 into CO using renewable H-2. Current ICCU-RWGS processes typically involve a gas-gas catalytic reaction whose efficiency is inherently limited by the Le Chatelier principle and side reactions. Here, we show a highly efficient ICCU process based on gas-solid carbonate hydrogenation using K promoted CaO (K-CaO) as a dual functional sorbent and catalyst. Importantly, this material allows similar to 100% CO2 capture efficiency during carbonation and bypasses the thermodynamic limitations of conventional gas-phase catalytic processes in hydrogenation of ICCU, achieving >95% CO2-to-CO conversion with similar to 100% selectivity. We showed that the excellent functionalities of the K-CaO materials arose from the formation of K2Ca(CO3)(2) bicarbonates with septal K2CO3 and CaCO3 layers, which preferentially undergo a direct gas-solid phase carbonates hydrogenation leading to the formation of CO, K2CO3 CaO and H2O. This work highlights the immediate potential of K-CaO as a class of dual-functional material for highly efficient ICCU and provides a new rationale for designing functional materials that could benefit the real-life application of ICCU processes.