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Selectivity control in hydrogenation through adaptive catalysis using ruthenium nanoparticles on a CO2-responsive support
Nature Chemistry ( IF 21.8 ) Pub Date : 2021-07-05 , DOI: 10.1038/s41557-021-00735-w
Alexis Bordet 1 , Sami El Sayed 2 , Matthew Sanger 3 , Kyle J Boniface 3 , Deepti Kalsi 1 , Kylie L Luska 2 , Philip G Jessop 3 , Walter Leitner 1, 2
Affiliation  

With the advent of renewable carbon resources, multifunctional catalysts are becoming essential to hydrogenate selectively biomass-derived substrates and intermediates. However, the development of adaptive catalytic systems, that is, with reversibly adjustable reactivity, able to cope with the intermittence of renewable resources remains a challenge. Here, we report the preparation of a catalytic system designed to respond adaptively to feed gas composition in hydrogenation reactions. Ruthenium nanoparticles immobilized on amine-functionalized polymer-grafted silica act as active and stable catalysts for the hydrogenation of biomass-derived furfural acetone and related substrates. Hydrogenation of the carbonyl group is selectively switched on or off if pure H2 or a H2/CO2 mixture is used, respectively. The formation of alkylammonium formate species by the catalytic reaction of CO2 and H2 at the amine-functionalized support has been identified as the most likely molecular trigger for the selectivity switch. As this reaction is fully reversible, the catalyst performance responds almost in real time to the feed gas composition.



中文翻译:

通过在 CO2 响应载体上使用钌纳米粒子的自适应催化控制加氢的选择性

随着可再生碳资源的出现,多功能催化剂对于选择性氢化生物质衍生的底物和中间体变得至关重要。然而,开发能够应对可再生资源间歇性的适应性催化系统,即具有可逆性可调节反应性的催化系统仍然是一个挑战。在这里,我们报告了一种催化系统的制备,该催化系统旨在自适应地响应加氢反应中的进料气体组成。固定在胺官能化聚合物接枝二氧化硅上的钌纳米粒子可作为生物质衍生的糠醛丙酮和相关底物加氢的活性和稳定催化剂。如果纯 H 2或 H 2 /CO 2则选择性地开启或关闭羰基的氢化分别使用混合物。通过 CO 2和 H 2在胺官能化载体上的催化反应形成烷基甲酸铵物质已被确定为选择性开关的最可能的分子触发因素。由于该反应是完全可逆的,因此催化剂性能几乎实时响应原料气组成。

更新日期:2021-07-05
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