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Identifying high-performance catalytic conditions for carbon dioxide reduction to dimethoxymethane by multivariate modelling

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Abstract

In times of a warming climate due to excessive carbon dioxide production, catalytic conversion of carbon dioxide to formaldehyde is not only a process of great industrial interest, but it could also serve as a means for meeting our climate goals. Currently, formaldehyde is produced in an energetically unfavourable and atom-inefficient process. A much needed solution remains academically challenging. Here we present an algorithmic workflow to improve the ruthenium-catalysed transformation of carbon dioxide to the formaldehyde derivative dimethoxymethane. Catalytic processes are typically optimised by comprehensive screening of catalysts, substrates, reaction parameters and additives to enhance activity and selectivity. The common problem of the multidimensionality of the parameter space, leading to only incremental improvement in laborious physical investigations, was overcome by combining elements from machine learning, optimisation and experimental design, tripling the turnover number of 786 to 2761. The optimised conditions were then used in a new reaction setup tailored to the process parameters leading to a turnover number of 3874, exceeding by far those of known processes.

Graphical abstract: Identifying high-performance catalytic conditions for carbon dioxide reduction to dimethoxymethane by multivariate modelling

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The article was received on 11 Sep 2019, accepted on 23 Oct 2019 and first published on 24 Oct 2019


Article type: Edge Article
DOI: 10.1039/C9SC04591K
Chem. Sci., 2019, Advance Article
  • Open access: Creative Commons BY license
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    Identifying high-performance catalytic conditions for carbon dioxide reduction to dimethoxymethane by multivariate modelling

    M. Siebert, G. Krennrich, M. Seibicke, A. F. Siegle and O. Trapp, Chem. Sci., 2019, Advance Article , DOI: 10.1039/C9SC04591K

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