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Review
. 2024 Oct 21;4(12):4546-4570.
doi: 10.1021/jacsau.4c00511. eCollection 2024 Dec 23.

Concatenating Microbial, Enzymatic, and Organometallic Catalysis for Integrated Conversion of Renewable Carbon Sources

Nina Klos  1   2 , Ole Osterthun  3 , Hendrik G Mengers  2 , Patrick Lanzerath  3 , William Graf von Westarp  4 , Guiyeoul Lim  2 , Marcel Gausmann  4 , Jan-Dirk Küsters-Spöring  1   2 , Jan Wiesenthal  3 , Nils Guntermann  3 , Lars Lauterbach  2 , Andreas Jupke  4   5 , Walter Leitner  3   6 , Lars M Blank  2 , Jürgen Klankermayer  3 , Dörte Rother  1   2
Affiliations
Review

Concatenating Microbial, Enzymatic, and Organometallic Catalysis for Integrated Conversion of Renewable Carbon Sources

Nina Klos et al. JACS Au. .

Abstract

The chemical industry can now seize the opportunity to improve the sustainability of its processes by replacing fossil carbon sources with renewable alternatives such as CO2, biomass, and plastics, thereby thinking ahead and having a look into the future. For their conversion to intermediate and final products, different types of catalysts-microbial, enzymatic, and organometallic-can be applied. The first part of this review shows how these catalysts can work separately in parallel, each route with unique requirements and advantages. While the different types of catalysts are often seen as competitive approaches, an increasing number of examples highlight, how combinations and concatenations of catalysts of the complete spectrum can open new roads to new products. Therefore, the second part focuses on the different catalysts either in one-step, one-pot transformations or in reaction cascades. In the former, the reaction conditions must be conflated but purification steps are minimized. In the latter, each catalyst can work under optimal conditions and the "hand-over points" should be chosen according to defined criteria like minimal energy usage during separation procedures. The examples are discussed in the context of the contributions of catalysis to the envisaged (bio)economy.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Various catalytic concepts.
Figure 2
Figure 2
Exemplary product synthesis route starting from CO2 with other C1 molecules as intermediates including the different catalyst types. Abbreviations: EDTA, ethylenediaminetetraacetic acid; PHA, polyhydroxyalkanoate; MTBE, methyl-tert-butyl ether.
Figure 3
Figure 3
Enzymatic three-step cascade from CO2 to methanol including cofactor recycling.
Figure 4
Figure 4
Oxygenation state of fuels versus biomass.
Figure 5
Figure 5
Overview of exemplary biomass-based feedstocks and products.
Figure 6
Figure 6
Chemical plastic usage.
Figure 7
Figure 7
Overview about the circular process from plastic waste for products. Abbreviations: PLA, polylactic acid; PS, polystyrole; PU, polyurethane; PET, polyethylene terephthalate.
Figure 8
Figure 8
Examples for combining different catalyst types in one-pot processes. (A) Combination of enzyme with microbe for the synthesis of (R)-3-hydroxyphenylacetylcarbinol ((R)-3-OH-PAC). (B) Combination of enzyme with organometallic catalyst starting from oleic acid to cycloheptene. (C) Combination of enzyme with electrocatalyst to use cellulose. (D) Combination of microbe with electrocatalyst to produce hydrogen and acetate or butyrate. (E) Combination of microbe with organometallic catalyst to produce stilbene and stilbene derivates.
Figure 9
Figure 9
Combining catalysts for improved atom economy in bioethanol fermentations.
Figure 10
Figure 10
Combining catalysts for novel biohybrid fuel production from biomass.
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