CE06 - Polymères, composites, physique et chimie de la matière molle, procédés

Supported Catalytically-Active Supramolecular Hydrogel for Flow Chemistry – CASH

Submission summary

This project deals with enzyme triggered self-assemblies of small peptides in polymer foams (supported Supramolecular Hydrogels). These hydrogels present catalytic activity resulting either from the peptide self-assembly itself, from enzymes embedded in the peptide self-assemblies or from both. In 2019, the two academic partners of this project have shown that such a supported Catalytically-Active Supramolecular Hydrogel (CASH) can lead to powerful catalytic continuous flow reactors. This pioneer work was patented (EP19306077, September 2019) and published recently (Angew. Chem., Int. Ed. 2019). The resulting hybrid material was mechanically robust and displayed a powerful esterase-like activity towards all classes of esters, a feature never reported so far using catalytic self-assemblies. But more interestingly, the enzyme used to form the catalytic hydrogel remained present and active in the material, opening the door of multiple and combined (bio)chemical transformations. In preliminary experiments, we have observed that the encapsulation of enzymes into the hydrogel increased their stability up to one year, expanding considerably the lifetime of the continuous flow process. This last aspect is highly interesting for an industrial technology transfer. Based on peptide design, molecular dynamics simulations, (bio)catalysis and chemical engineering investigations, our goal here is to design original and top-performing catalytic phases for flow developments based on our supported-CASH strategy, highlighting so the potential of this approach for industrial applications. Two types of CASH will be developed: (i) CASH whose catalytic activity originates from the peptide self-assembly itself (called SA way) and (ii) CASH whose catalytic activity comes from enzymes encapsulated in the peptide self-assembly architecture (called E way)
First, this project aims to establish a general peptide sequence suitable to design a large variety of supported-CASH exhibiting various catalytic activities. Aldolization is targeted to illustrate the potential of our peptide design strategy. Second, we will develop a universal method to encapsulate all kinds of enzyme in supramolecular hydrogels leading to enzymatically active materials to fulfill tubular flow reactors (E way). In collaboration with ALYSOPHIL, our industrial partner expert in flow chemistry, we will develop a gram scale reactor and apply our technology from either SA or E way and apply it to compounds of industrial interest. In order to control the design and use of various supported CASH, fundamental investigations will be performed both experimentally and using molecular dynamic computer simulations. We will address issues such as the mechanism of the self-assembly process initiated at enzymes, the dynamics of the enzymes in the self-assembled hydrogel (mobility, thermodynamic equilibrium between enzymes bound to the self-assembly and free enzymes), mechanical properties of the resulting CASH and its stability when brought in contact with water/solent mixtures.
This project is a “PRCE” going from TRL1 to TRL5. Our goal is to keep our scientific leading position and to transfer to industry our discoveries to produce valuable compounds through a highly competitive process. Thanks to flow chemistry, we are going to seek energy saving, yield and selectivity increase as well as production costs reduction. These are current key challenges faced by industry and requested by the society.

Project coordination

Loïc Jierry (Institut Charles Sadron (UPR 22))

The author of this summary is the project coordinator, who is responsible for the content of this summary. The ANR declines any responsibility as for its contents.

Partner

BioMat Biomatériaux et bioingénierie (UMR_S 1121)
CMC Chimie de la Matière Complexe (UMR 7140)
ALYSOPHIL
I.C.S Institut Charles Sadron (UPR 22)

Help of the ANR 465,790 euros
Beginning and duration of the scientific project: - 42 Months

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