Periodic Reporting for period 1 - SMARTBOX (Selective Modifications of ARomatics through Biocatalytic Oxidations)
Reporting period: 2019-05-01 to 2020-10-31
Relying on the advanced engineering platform, SMARTBOX will develop the one-enzyme conversion of HMF into FDCA and intermediates, and the one-enzyme conversion of lignin monomers into a potential biobased building block for polycarbonates and vanillin. By adopting a one-enzyme FDCA production process, the associated production costs and carbon footprint are expected to decrease significantly compared to SOTA chemical oxidation methods. The unique feature of SMARTBOX is that reductive catalytic fractionation (RCF) will be used to selectively produce specific lignin monomers from biomass in near theoretical yields. The structural similarity of the resulting monomers with the SMARTBOX building blocks allows the development of high-yielding processes with only one enzyme. Due to the smart combination between oxidative biocatalysis and RCF, the production of added-value bio-aromatics will proceed with higher yields than the state of the art.
There are 2 publications for the intermediates development through reductive catalytic fractionation (RCF) by KUL ((i) on developed solvent extraction protocols that have generated ‘simplified oil fractions’ DOI: 10.1039/D0SC04182C) in the high impact Journal of Chemical Sciences, and (ii) on pending challenges of biorefinery reactor/process technology and scalability summarized in an opinion article (DOI.org/10.1021/acs.iecr.0c02294)) and some more are in the pipeline for the enzyme engineering through the ‘Framework for Rapid Enzyme Stabilization by Computational libraries’ (FRESCO) and Zymvolver platform.
The in silico FRESCO computational method (Wiljma et al 2014) was applied successfully by partners (RUG/Zymvol) to several oxidative enzymes to improve the stability of these enzymes and increase the resistance to co-solvents. For the first application turning HMF into FDCA the best candidates resulting from an HMFO mutant library generated by computational design (ZYMVOL) was screened by RUG. The industrial production up to 150L scale of enzymatic FDCA via bioconversion and its following purification steps was done successfully by BBEPP, making the bio-based building block available at high polymer grade purity and in bigger quantities.
The selective production of specific lignin monomers through RCF is successfully done at lab-scale and first intermediates have been send to partners for enzymatic conversion experiments. The basic design of the prototype for the mini-pilot reactor to produce intermediates on kg scale has been finished.
The framework of the sustainability and risk assessment with a common basis for the evaluation of the investigated SMARTBOX technologies has been defined, including (i) the goal and scope definition, value chain definition with a short description of the processes, identification of boundaries for the different assessments and (ii) the description of the methodologies used for the LCA/ TEA.
At this point in the project, we can state that the enzymatic production of FDCA via bioconversion at 150L scale and purification towards a purity higher than the benchmark chemical FDCA is the most significant technological achievement. This achievement can be labelled as a breakthrough step as before the start of the project, biocatalytic processes that converted HMF into FDCA had only been performed at lab-scale. The objective of producing PEF with FDCA obtained by enzymatic bioconversion is still relevant as it shows that bioconversion can be used to produce polymer grade FDCA which could provide scientific and technological breakthrough potential.
The developed solvent extraction protocols have generated ‘simplified oil fractions’ which led to a beyond-the-state-of-the-art understanding of the structure of complex lignin molecules in the RCF oil. The results have been published in the high impact Journal of Chemical Sciences and will provide valuable information for both the scientific community as well as interested industry, for instance to link structural motives to specific product properties.
Extensive collaboration and discussions with the engineering firm during basic design of the planned pilot-scale RCF reactor (needed to reach TRL5), as well as discussions with TRANSfarm, the host location of the pilot reactor, has led to new insights about the pending challenges of biorefinery reactor/process technology and scalability. This knowledge is used by KUL to steer its own research activities, but has also been summarized in an opinion article in the Journal Industrial & Engineering Chemistry Research, to steer the activities of the broader scientific community around lignin and biorefinery research and development.
SMARTBOX will provide a TEA, LCA and Natural and Social Capital Valuation assessment of the four value chains investigated, from raw material extraction to related end-use products. The advantages in terms of sustainability, technology and economy will be compared with the current available state-of-the-art technology, providing a complete picture of the benefits of SMARTBOX.