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Controlling CO2 Hydrogenation Selectivity by Metal-Supported Electron Transfer |
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| Authors: | Xiaoyu Li Dr. Jian Lin Prof. Lin Li Yike Huang Xiaoli Pan Sebastián E. Collins Yujing Ren Yang Su Dr. Leilei Kang Prof. Xiaoyan Liu Yanliang Zhou Hua Wang Prof. Aiqin Wang Prof. Botao Qiao Prof. Xiaodong Wang Prof. Tao Zhang |
| Affiliation: | 1. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China University of Chinese Academy of Sciences, 100049 Beijing, China;2. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China;3. Instituto de Desarrollo Tecnológico para la Industria Química (INTEC), Universidad Nacional del Litoral, CONICET, Güemes 3450, S3000GLN Santa Fe, Argentina;4. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China |
| Abstract: | Tuning CO2 hydrogenation selectivity to obtain targeted value-added chemicals and fuels has attracted increasing attention. However, a fundamental understanding of the way to control the selectivity is still lacking, posing a challenge in catalyst design and development. Herein, we report our new discovery in ambient pressure CO2 hydrogenation reaction where selectivity can be completely reversed by simply changing the crystal phases of TiO2 support (anatase- or rutile-TiO2) or changing metal loadings on anatase-TiO2. Operando spectroscopy and NAP-XPS studies reveal that the determining factor is a different electron transfer from metal to the support, most probably as a result of the different extents of hydrogen spillover, which changes the adsorption and activation of the intermediate of CO. Based on this new finding, we can not only regulate CO2 hydrogenation selectivity but also tune catalytic performance in other important reactions, thus opening up a door for efficient catalyst development by rational design. |
| Keywords: | CO2 crystal phase electron transfer hydrogen spillover selectivity |