A Multi-Enzyme Cascade for the Production of High-Value Aromatic Compounds

Engelmann, Claudia; Johannsen, Jens; Waluga, Thomas; Fieg, Georg; Liese, Andreas; Bubenheim, Paul

doi:10.3390/catal10101216

Cited by 13 publications

(21 citation statements)

References 46 publications

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“…Especially in the last 800 min of the experiment, the experimentally determined molar balance varies: this can be due to dead volume in the organic cycle containing xylene, leading to a dilution of the samples or precipitation of the components CAL, COH, or CAC. Potential side reactions behind such variations have not been observed 26 . It shall be noted that the variations in overall molar balance are significantly smaller for the other experiments, ranging from 5.98 to 17.68%, as can be seen in the Supporting Information.…”

Section: Model Validationmentioning

confidence: 79%

“…A bi-bi mechanism with competitive inhibition for both the ADHcatalyzed reaction of cinnamyl aldehyde (CAL) to cinnamyl alcohol (COH) and the FDH-catalyzed reaction of formate to CO 2 are implemented in the model according to initial rate measurements as presented by Engelmann et al, 26 describing the ADH reaction rate according to Equation (1) and the FDH reaction rate according to Equation (2). The corresponding values for the constants are listed in Table 1.…”

Section: Aqueous Phasementioning

confidence: 99%

“…A bi‐bi mechanism with competitive inhibition for both the ADH‐catalyzed reaction of cinnamyl aldehyde (CAL) to cinnamyl alcohol (COH) and the FDH‐catalyzed reaction of formate to CO 2 are implemented in the model according to initial rate measurements as presented by Engelmann et al, 26 describing the ADH reaction rate according to Equation ) and the FDH reaction rate according to Equation ). The corresponding values for the constants are listed in Table 1.

v_{ADH} = \frac{v_{\max, ADH} ∙ ((), ([], CAL) ∙ ([], NADH))}{\begin{matrix} K_{normalm, CAL} ∙ K_{normalm, NADH + H^{+}} ∙ ((), 1 + \frac{[COH]}{K_{I, COH}}) + K_{normalm, NADH} ∙ ([], CAL) \\ + K_{normalm, CAL} ∙ ([], NADH) ∙ ((), 1 + \frac{[COH]}{K_{I, COH}}) + ([], CAL) ∙ ([], NADH) \end{matrix}}

v_{FDH} = \frac{v_{\max, FDH} ∙ ((), ([], {NAD}^{+}) ∙ ([], formate))}{\begin{matrix} K_{normalm, NAD} ∙ K_{normalm, formate} ∙ ((), 1 + \frac{[NADH]}{K_{I, NADH}}) + K_{normalm, formate} ∙ ([], {NAD}^{+}) \\ + K_{normalm, {NAD}^{+}} ∙ ([], formate) ∙ ((), 1 + \frac{[NADH]}{K_{I, NADH}}) + ([], formate) ∙ ([], {NAD}^{+}) \end{matrix}}

…”

Section: Mathematical Modelmentioning

confidence: 99%

“…Since component precipitation in the organic‐phase cycle was not noted due to the high saturation concentrations of the cinnamyl derivatives, no storage term is implemented in this sub‐model. Based on progress curve analyses described by Engelmann et al, 26 the lipase reaction rate is described according to a bi‐bi mechanism with substrate excess inhibition of CAC for the present reaction system. Equation ) shows the lipase reaction rate as implemented in the model, and the corresponding parameters are described in Table 3 32…”

Section: Mathematical Modelmentioning

confidence: 99%

“…In Figure 4 Throughout all six experiments we simulated for model validation, the mean deviation reached values of 26.0% and 22.6% for COH and CCI respectively, and 11.66% for the overall molar balance, which can be traced back to the deviations of the enzymes' kinetic parameters. 26,[33][34][35] In literature, mathematical models for such complex multienzyme processes across phase boundaries in miniplant-scale and continuous operation cannot be found to the best of our knowledge.…”

Section: Model Validationmentioning

confidence: 99%

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Multi‐enzyme cascade reaction in a miniplant two‐phase‐system: Model validation and mathematical optimization

et al. 2021

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Biotechnological application of multiple enzymes in different phases for target compounds synthesis poses a significant challenge for industrial process development. At the same time, a growing demand for natural flavors and fragrances opens up possibilities for novel biotechnological processes to replace current chemical synthesis routes, with additional advantages such as avoiding harsh reaction conditions and toxic chemicals, and less by-products in the system. Within complex biotechnological processes, the key for unfolding their industrial application potential in bioprocess engineering lies in their mathematical modeling. In this contribution, a multi-enzyme cascade reaction in a two-phase system implemented in a miniplant-scale reactor setup is mathematically modeled for the example of the flavoring agent cinnamyl cinnamate. Using our validated model and a mathematical optimization tool based on a genetic algorithm, optimization runs are performed to demonstrate the potential of computer-aided process development for complex biotechnological processes.

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Section: Model Validationmentioning

confidence: 79%

Section: Aqueous Phasementioning

confidence: 99%

v_{ADH} = \frac{v_{\max, ADH} ∙ ((), ([], CAL) ∙ ([], NADH))}{\begin{matrix} K_{normalm, CAL} ∙ K_{normalm, NADH + H^{+}} ∙ ((), 1 + \frac{[COH]}{K_{I, COH}}) + K_{normalm, NADH} ∙ ([], CAL) \\ + K_{normalm, CAL} ∙ ([], NADH) ∙ ((), 1 + \frac{[COH]}{K_{I, COH}}) + ([], CAL) ∙ ([], NADH) \end{matrix}}

v_{FDH} = \frac{v_{\max, FDH} ∙ ((), ([], {NAD}^{+}) ∙ ([], formate))}{\begin{matrix} K_{normalm, NAD} ∙ K_{normalm, formate} ∙ ((), 1 + \frac{[NADH]}{K_{I, NADH}}) + K_{normalm, formate} ∙ ([], {NAD}^{+}) \\ + K_{normalm, {NAD}^{+}} ∙ ([], formate) ∙ ((), 1 + \frac{[NADH]}{K_{I, NADH}}) + ([], formate) ∙ ([], {NAD}^{+}) \end{matrix}}

…”

Section: Mathematical Modelmentioning

confidence: 99%

Section: Mathematical Modelmentioning

confidence: 99%

Section: Model Validationmentioning

confidence: 99%

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Multi‐enzyme cascade reaction in a miniplant two‐phase‐system: Model validation and mathematical optimization

et al. 2021

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Multienzymatic Cascades and Nanomaterial Scaffolding—A Potential Way Forward for the Efficient Biosynthesis of Novel Chemical Products

Hooe,

Smith,

Dean

et al. 2023

Advanced Materials

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Synthetic biology is touted as the next industrial revolution as it promises access to greener biocatalytic syntheses to replace many industrial organic chemistries. Here, it is shown to what synthetic biology can offer in the form of multienzyme cascades for the synthesis of the most basic of new materials—chemicals, including especially designer chemical products and their analogs. Since achieving this is predicated on dramatically expanding the chemical space that enzymes access, such chemistry will probably be undertaken in cell‐free or minimalist formats to overcome the inherent toxicity of non‐natural substrates to living cells. Laying out relevant aspects that need to be considered in the design of multi‐enzymatic cascades for these purposes is begun. Representative multienzymatic cascades are critically reviewed, which have been specifically developed for the synthesis of compounds that have either been made only by traditional organic synthesis along with those cascades utilized for novel compound syntheses. Lastly, an overview of strategies that look toward exploiting bio/nanomaterials for accessing channeling and other nanoscale materials phenomena in vitro to direct novel enzymatic biosynthesis and improve catalytic efficiency is provided. Finally, a perspective on what is needed for this field to develop in the short and long term is presented.

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Liquid‐Liquid Centrifugal Extractors: Types and Recent Applications – a Review

Hamamah

Grützner

2022

ChemBioEng Reviews

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In light of the elevating pressures toward adopting intensifying technologies, centrifugal extractors are increasingly drawing attention as a promising alternative to traditional extraction equipment. Recently, many fields have applied them in research and that resulted in a considerable amount of information that may be hard to follow. To keep interested researchers updated, this work presents the state‐of‐the‐art status of those devices. That is, the different types of centrifugal extractors are first surveyed with emphasis on those available on the market nowadays. Then, their recent applications are covered with exclusion of two fields: oil‐water separations and nuclear industry, as the purpose is to accent centrifugal extractors' potential and compatibility with the widest possible range of applications beyond traditional ones. A further section addresses the hydrodynamics of annular centrifugal contactors that form a major subfamily of centrifugal extractors. Those annular variants have received special focus throughout this work, since not only are they the most encountered devices in literature but also still to date under development with latest versions being 3D‐printed.

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A Multi-Enzyme Cascade for the Production of High-Value Aromatic Compounds

Cited by 13 publications

References 46 publications

Multi‐enzyme cascade reaction in a miniplant two‐phase‐system: Model validation and mathematical optimization

Multi‐enzyme cascade reaction in a miniplant two‐phase‐system: Model validation and mathematical optimization

Multienzymatic Cascades and Nanomaterial Scaffolding—A Potential Way Forward for the Efficient Biosynthesis of Novel Chemical Products

Liquid‐Liquid Centrifugal Extractors: Types and Recent Applications – a Review

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