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Steering CO2 hydrogenation toward C-C coupling to hydrocarbons using porous organic polymer/metal interfaces.


ABSTRACT: The conversion of CO2 into fuels and chemicals is an attractive option for mitigating CO2 emissions. Controlling the selectivity of this process is beneficial to produce desirable liquid fuels, but C-C coupling is a limiting step in the reaction that requires high pressures. Here, we propose a strategy to favor C-C coupling on a supported Ru/TiO2 catalyst by encapsulating it within the polymer layers of an imine-based porous organic polymer that controls its selectivity. Such polymer confinement modifies the CO2 hydrogenation behavior of the Ru surface, significantly enhancing the C2+ production turnover frequency by 10-fold. We demonstrate that the polymer layers affect the adsorption of reactants and intermediates while being stable under the demanding reaction conditions. Our findings highlight the promising opportunity of using polymer/metal interfaces for the rational engineering of active sites and as a general tool for controlling selective transformations in supported catalyst systems.

SUBMITTER: Zhou C 

PROVIDER: S-EPMC8851537 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Steering CO<sub>2</sub> hydrogenation toward C-C coupling to hydrocarbons using porous organic polymer/metal interfaces.

Zhou Chengshuang C   Asundi Arun S AS   Goodman Emmett D ED   Hong Jiyun J   Werghi Baraa B   Hoffman Adam S AS   Nathan Sindhu S SS   Bent Stacey F SF   Bare Simon R SR   Cargnello Matteo M  

Proceedings of the National Academy of Sciences of the United States of America 20220201 7


The conversion of CO<sub>2</sub> into fuels and chemicals is an attractive option for mitigating CO<sub>2</sub> emissions. Controlling the selectivity of this process is beneficial to produce desirable liquid fuels, but C-C coupling is a limiting step in the reaction that requires high pressures. Here, we propose a strategy to favor C-C coupling on a supported Ru/TiO<sub>2</sub> catalyst by encapsulating it within the polymer layers of an imine-based porous organic polymer that controls its sele  ...[more]

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