Boosting of enzymatic cascades by intermediates: Theoretical analysis and model-based optimization DOI Creative Commons
Leandros Paschalidis,

Daniela Fröschl,

Manuel Plana

et al.

Biochemical Engineering Journal, Journal Year: 2024, Volume and Issue: 210, P. 109440 - 109440

Published: July 27, 2024

A recent paper demonstrated that adding intermediates of an enzymatic cascade reaction at the start process can increase space-time yield significantly. This method was coined boosting by (BBI) and potentially productivity systems. BBI remains largely unexplored, its mechanism, potential, limitations are not fully understood. In this short communication, theoretical background is revealed studying four chemical networks exhibit through intermediates. The dynamics these studied via quasi-steady state approximation numerical solutions. novel graphical be used to deduce which boost linear, redox-neutral presented. Further, how such a designed using model-based optimization demonstrated.

Language: Английский

Bayesian Optimization for an ATP-Regenerating In Vitro Enzyme Cascade DOI Open Access
Regine Siedentop, Maximilian Siska, Niklas Möller

et al.

Catalysts, Journal Year: 2023, Volume and Issue: 13(3), P. 468 - 468

Published: Feb. 23, 2023

Enzyme cascades are an emerging synthetic tool for the synthesis of various molecules, combining advantages biocatalysis and one-pot multi-step reactions. However, more complex enzyme cascade is, difficult it is to achieve adequate productivities product concentrations. Therefore, whole process must be optimized account synergistic effects. One way deal with this challenge involves data-driven models in combination experimental validation. Here, Bayesian optimization was applied ATP-producing -regenerating consisting polyphosphate kinases. The co-substrate concentrations were adjusted ATP-dependent reaction, catalyzed by mevalonate kinase (MVK). With a total 16 experiments, we able iteratively optimize initial components used improve specific activity MVK 10.2 U mg−1. even exceeded results reference reaction stoichiometrically added ATP amounts, which 8.8 mg−1 reached. At same time, also improved so that complete yields achieved.

Language: Английский

Citations

13

Modeling Enzymatic Cascade Reactions Immobilized in Plug‐Flow Reactors for Flow Biocatalysis DOI Creative Commons
Leandros Paschalidis, Sara Arana‐Peña, Volker Sieber

et al.

Chemie Ingenieur Technik, Journal Year: 2024, Volume and Issue: 96(6), P. 741 - 748

Published: April 16, 2024

Abstract Flow biocatalysis has emerged as a promising technology for the sustainable production of chemicals. Multiple immobilized enzymes are often used biocatalysts to perform enzymatic cascade reactions in flow biocatalytic systems. When designing packed‐bed reactors with multiple enzymes, distributed porous particles, and particles catalyst zones. A recently developed methodology is extended selecting spatial immobilization distributions batch reactors. Mechanistic models compare three most basic designs reactor, i.e., mixed individually separated co‐immobilized enzymes. For first‐order microkinetics, design was found always outperform other two. Separating two zones proven mixing them one zone any positive order reaction kinetic.

Language: Английский

Citations

1

Using Adsorption Energy Distribution for Parameter Estimation of Competitive Cofactor Coupled Enzyme Reaction DOI Open Access
Thomas Waluga, Mirko Skiborowski

Processes, Journal Year: 2023, Volume and Issue: 11(9), P. 2686 - 2686

Published: Sept. 7, 2023

The chemical and biotechnology industries are facing new challenges in the use of renewable resources. complex nature these materials requires advanced techniques to understand kinetics reactions this context. This study presents an interdisciplinary approach analyze cofactor coupled enzymatic two-substrate competitive a fast efficient manner. By studying adsorption energy distribution (AED), it is possible determine individual parameters reaction kinetics. In case single alcohol reaction, AED able identify agreement with literature few experimental data points compared classical methods. analysis can automatically number competing substrates, whereas traditional nonlinear regression prior knowledge information for parameter identification.

Language: Английский

Citations

2

Reaction Engineering and Comparison of Electroenzymatic and Enzymatic ATP Regeneration Systems DOI Creative Commons
Regine Siedentop, Tobias Prenzel, Siegfried R. Waldvogel

et al.

ChemElectroChem, Journal Year: 2023, Volume and Issue: 10(22)

Published: Oct. 5, 2023

Abstract Adenosine‐5’‐triphosphate (ATP) plays a crucial role in many biocatalytic reactions and its regeneration can influence the performance of related enzymatic reaction significantly. Here, we established electrochemically coupled ATP by pyruvate oxidase acetate kinase (ACK) for phosphorylation mevalonate catalyzed kinase. A yield 84 % product phosphate was reached total turnover number ADP 68. These metrics are promising development an economic feasible bioprocess surpass other systems. comparison made to polyphosphate kinases (PPKs), ACK, kinase, creatine terms donor properties exemplary reactions. Furthermore, our system expanded PPK that enables AMP, which broaden spectrum applications even further.

Language: Английский

Citations

2

Boosting of Enzymatic Cascades by Intermediates: Theoretical Analysis and Model-Based Optimization DOI
Leandros Paschalidis,

Daniela Fröschl,

Manuel Plana

et al.

Published: Jan. 1, 2024

In an earlier work we demonstrated that adding intermediates of enzymatic cascade reaction at the start process can increase space-time yield significantly. This method was coined boosting by (BBI) and potentially productivity systems. BBI remains largely unexplored, its mechanism, potential, limitations are not fully understood. present work, provide a theoretical background studying four chemical networks (CRN) exhibit intermediates. We study dynamics these via quasi steady-state approximation numerical solutions. novel graphical be used to deduce which boost linear, redox neutral networks. Further, demonstrate how such designed using model-based optimization.

Language: Английский

Citations

0

Boosting of enzymatic cascades by intermediates: Theoretical analysis and model-based optimization DOI Creative Commons
Leandros Paschalidis,

Daniela Fröschl,

Manuel Plana

et al.

Biochemical Engineering Journal, Journal Year: 2024, Volume and Issue: 210, P. 109440 - 109440

Published: July 27, 2024

A recent paper demonstrated that adding intermediates of an enzymatic cascade reaction at the start process can increase space-time yield significantly. This method was coined boosting by (BBI) and potentially productivity systems. BBI remains largely unexplored, its mechanism, potential, limitations are not fully understood. In this short communication, theoretical background is revealed studying four chemical networks exhibit through intermediates. The dynamics these studied via quasi-steady state approximation numerical solutions. novel graphical be used to deduce which boost linear, redox-neutral presented. Further, how such a designed using model-based optimization demonstrated.

Language: Английский

Citations

0