Li Xiaoyu, Lin Jian, Li Lin, Huang Yike, Pan Xiaoli, Collins Sebastián E, Ren Yujing, Su Yang, Kang Leilei, Liu Xiaoyan, Zhou Yanliang, Wang Hua, Wang Aiqin, Qiao Botao, Wang Xiaodong, Zhang Tao
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.
Angew Chem Int Ed Engl. 2020 Nov 2;59(45):19983-19989. doi: 10.1002/anie.202003847. Epub 2020 Aug 31.
Tuning CO 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 CO hydrogenation reaction where selectivity can be completely reversed by simply changing the crystal phases of TiO support (anatase- or rutile-TiO ) or changing metal loadings on anatase-TiO . 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 CO hydrogenation selectivity but also tune catalytic performance in other important reactions, thus opening up a door for efficient catalyst development by rational design.
调节CO加氢选择性以获得目标增值化学品和燃料已引起越来越多的关注。然而，目前仍缺乏对控制选择性方法的基本理解，这给催化剂的设计和开发带来了挑战。在此，我们报告了在常压CO加氢反应中的新发现，即通过简单地改变TiO载体的晶相（锐钛矿型或金红石型TiO）或改变锐钛矿型TiO上的金属负载量，可以使选择性完全反转。原位光谱和NAP-XPS研究表明，决定因素是金属向载体的不同电子转移，很可能是由于氢溢流程度不同，这改变了CO中间体的吸附和活化。基于这一新发现，我们不仅可以调节CO加氢选择性，还可以调节其他重要反应中的催化性能，从而为通过合理设计进行高效催化剂开发打开了一扇门。
