Article
Chemistry, Multidisciplinary
Max Lubberink, William Finnigan, Christian Schnepel, Christopher R. Baldwin, Nicholas J. Turner, Sabine L. Flitsch
Summary: A biocatalytic route towards N-alkanoyl-N-methylglucamides (MEGAs) and analogues was developed using a modified carboxylic acid reductase construct (CARmm-A). The selective formation of amide bonds was achieved without competing reactions. Reaction optimization resulted in reduced amine concentration requirements, enabling efficient amide formation. The wide substrate scope of CARmm-A was demonstrated through the synthesis of 24 commercially relevant amides.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Max Lubberink, William Finnigan, Sabine L. Flitsch
Summary: Amide bonds are commonly formed in the pharmaceutical industry and there is a growing interest in biocatalytic methods for their synthesis. The use of low water systems and ATP-dependent enzymes have shown promise in driving amide bond formation. A publicly available database, RetroBioCat, has been compiled to provide literature on these methods.
Article
Polymer Science
Peter Kei, Mitchell T. Howell, Carlos A. Chavez, Joseph C. Mai, Changwoo Do, Kunlun Hong, Evgueni E. Nesterov
Summary: Conjugated polymer materials possess highly complex structures that can span several orders of magnitude in length scale, influenced by weak secondary interactions and entropic forces. Understanding the molecular interactions is crucial for the design and development of condensed CP materials, especially for systems away from equilibrium. A promising approach for accessing various kinetically stabilized semi-crystalline CP nanostructures involves controlled chain-growth polymerization initiated by small-molecule catalytic species. The resulting hierarchically organized semi-crystalline CP systems offer a range of optoelectronic properties, with structural aspects revealed through advanced techniques like X-ray diffraction and neutron scattering.
Article
Chemistry, Multidisciplinary
Mengyun Chen, Tiankai Zhang, Anna Elsukova, Zhangjun Hu, Rui Zhang, Yonghong Wang, Xianjie Liu, Xiaoke Liu, Feng Gao
Summary: Stable CsPbI3 nanoplatelets with lower surface-area-to-volume ratio and improved spectral stability are synthesized by accelerating the crystallization process using kinetic control.
Article
Chemistry, Multidisciplinary
Andreea Veronica Dediu Botezatu, Gabriela Elena Bahrim, Claudia Veronica Ungureanu, Anna Cazanevscaia Busuioc, Bianca Furdui, Rodica Mihaela Dinica
Summary: An efficient one-pot route leading to bis-indolizine symmetric compounds has been developed using a new approach involving biocatalysis. The biocatalysts showed good catalytic potential and led to moderate to excellent yields of the target compounds. Horseradish root was found to be the most promising biocatalyst source, providing higher yields compared to the conventional synthesis method. The structures of the indolizine derivatives were confirmed using various analytical techniques. The obtained compounds exhibited low cytotoxicity on the growth of yeast cells.
GREEN PROCESSING AND SYNTHESIS
(2023)
Article
Engineering, Environmental
Xi-Jie Lin, Yong-Gang Sun, Si-Jie Guo, Si-Dong Zhang, Yuan Liu, An-Min Cao
Summary: Switching to anhydrous solution allows for the construction of uniform Fe2O3 nanoshells without the involvement of corrosive environment. By using hexamethylenetetramine as a growth controller, the growth kinetics of the formed metal hydroxide precursor can be modulated, resulting in core@shell structures with controlled shell thickness at nanometer accuracy. This synthetic protocol is successful in building uniform Fe2O3 coatings around various substrates, particularly LiNi0.5Mn1.5O4, improving the electrochemical behavior and high temperature stability of the cathode.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Junlong Liao, Cun Zhu, Zhenzhu He, Junning Zhang, Yi Zeng, Zhongze Gu
Summary: We report a versatile approach to fabricate nonspherical polystyrene nanoparticles with controlled morphologies based on kinetically controlled seed-mediated polymerization. By manipulating reaction kinetics parameters, such as monomer concentration, reactant injection rate, and reaction temperature, we can direct the monomers to polymerize on selective sites of PS seeds, resulting in nonspherical nanoparticles with various thermodynamically unfavored morphologies. The formation mechanism of these nanoparticles has been systematically investigated by monitoring seed evolution during the reaction. This method has also been successfully extended to different monomer and seed systems.
Article
Agriculture, Multidisciplinary
Haixia Xu, Xiaofeng Li, Xuan Xin, Lan Mo, Yucong Zou, Guanglei Zhao, Yigang Yu, Kebing Chen
Summary: In this study, a green solvent system was developed to synthesize arbutin esters with improved liposolubilities, among which arbutin undecenoate (AU) showed the strongest tyrosinase-inhibiting activity compared to arbutin. AU was found to be a competitive inhibitor with reversible inhibition, with its mechanism of tyrosinase inhibition involving making the secondary structure of the enzyme looser and less stable. Additionally, AU significantly reduced melanin content in B16 mouse melanoma cells.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Thien-Kim Le, Jinhyun Kim, Ngoc Anh Nguyen, Thi Huong Ha Nguyen, Eun-Gene Sun, Su-Min Yee, Hyung-Sik Kang, Soo-Jin Yeom, Chan Beum Park, Chul-Ho Yun
Summary: Photobiocatalysis is a green platform for driving redox enzymatic reactions using solar energy without high-cost cofactors. Natural flavins were used as photosensitizers to develop a visible light-driven whole-cell platform for human cytochrome P450 (CYP) photobiocatalysis. The research showed that flavins can mediate light-driven biocatalysis by human CYPs in whole-cell systems, demonstrating the general applicability of solar-powered P450 photobiocatalytic system.
Article
Agricultural Engineering
Qiang Chen, Mingzhao Guo, Yuexin Bi, Ge Qu, Zhoutong Sun, Yujun Wang, Guangsheng Luo
Summary: This study achieved efficient synthesis of S-(4-chlorophenyl)-(pyridin-2-yl) methanol (S-CPMA) by using recombinant Escherichia coli as a whole-cell catalyst and developing a microreaction system. This approach reduced the reaction time and increased the yield by over 70%.
BIORESOURCE TECHNOLOGY
(2021)
Article
Chemistry, Applied
Marc Devillard, Carlos Antonio De Albuquerque Pinheiro, Elsa Caytan, Claire Roiland, Chiara Dinoi, Iker Del Rosal, Gilles Alcaraz
Summary: This study reveals the uncatalyzed formation of polyaminoboranes from monomeric diisopropylaminoborane and primary amines, with a detailed investigation on their structure and reaction mechanism. The presence of magnetically non-equivalent methylenic protons near the BN-backbone in N-alkyl substituted PABs is also highlighted. It is shown through DFT calculations that the formation of polyaminoboranes results from a kinetically controlled step-growth polymerization reaction.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Chemistry, Physical
Jiyu Tian, Eli Zysman-Colman, Finlay D. Morrison
Summary: The study investigates the formation of partial solid solutions in Az(1-x)FA(x)PbBr(3) using similar-sized cations Az(+) and FA(+). Results show a clear mismatch in composition between precipitated samples and corresponding solutions, indicating kinetic control during precipitation compared to mechanosynthesis. Additionally, it is found that FA(+) is smaller than Az(+), contradicting existing literature.
CHEMISTRY OF MATERIALS
(2021)
Review
Biotechnology & Applied Microbiology
Behnaz Nowrouzi, Leonardo Rios-Solis
Summary: The increasing trend towards producing cytochrome P450-mediated natural products in microbial systems is due to the challenging nature of organic chemistry methods. Manipulating the redox potential in microbial chassis for natural product synthesis is limited, as the crucial role of redox state in regulating P450 biocatalysis has been underestimated.
CRITICAL REVIEWS IN BIOTECHNOLOGY
(2022)
Review
Biotechnology & Applied Microbiology
Robin Dorau, Peter Ruhdal Jensen, Christian Solem
Summary: There is a growing demand for lactose-free dairy products worldwide, with discussions on the characteristics of lactase enzymes and the potential of whole-cell lactase catalysts. Lactic acid bacteria appear to be optimal candidates, but face technical hurdles in industrial exploitation.
APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
(2021)
Article
Chemistry, Applied
Suman Maji, Sukumar Pradhan, Karishma Pidiyara, Siddhartha Maiti, Shaeel A. Al-Thabaiti, Debabrata Maiti
Summary: This work presents a palladium(II)-catalyzed regioselective C8-H olefination of 1-naphthamides. Notably, naphthamide fused lactam 2,3-dihydro-1H-benzo[de]isoquinolin-1-one derivatives were synthesized in a particular class of napthamides. The reaction showed good compatibility with a diverse range of acrylates and styrenes, providing the desired products with high yields and tolerance to various functional groups. The developed strategy was further employed for the synthesis of different drug derivatives.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Biochemical Research Methods
Diego Salamanca, Katja Buehler, Karl-Heinrich Engesser, Andreas Schmid, Rohan Karande
Summary: This study investigates the use of an Acidovorax mutant as a whole-cell biocatalyst for converting cycloalkanes to omega-hydroxycarboxylic acids, showcasing high metabolic efficiency with an efficient enzyme cascade. The deletion of a specific enzyme in the metabolic pathway led to the production of short-chain omega-hydroxycarboxylic acids, demonstrating a high molar conversion rate above 98% within 6 hours.
Article
Biotechnology & Applied Microbiology
Lisa Bretschneider, Martin Wegner, Katja Buehler, Bruno Buehler, Rohan Karande
Summary: A bioprocess for synthesizing 6-aminohexanoic acid (6AHA) was developed using a mixed-species approach with promising results. The combination of Pseudomonas taiwanensis and Escherichia coli strains allowed for high conversion and yield of 6AHA under environmentally benign conditions.
MICROBIAL BIOTECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Konstantin Wink, Marie van Der Loh, Nora Hartner, Matthias Polack, Christian Dusny, Andreas Schmid, Detlev Belder
Summary: Chemically specific and quantifiable monitoring of biocatalytic transformations at the single-cell level has been achieved through the integration of droplet microfluidics, cell imaging, and mass spectrometry.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biotechnology & Applied Microbiology
Marcel Grund, Torsten Jakob, Joerg Toepel, Andreas Schmid, Christian Wilhelm, Bruno Buehler
Summary: Previous studies have reported various effects of heterologous production of carbon-based molecules on photosynthetic and growth efficiency of cyanobacteria. However, the use of batch cultivation and continuously changing growth conditions hindered the clear differentiation between the impact of cultivation conditions on cell physiology and effects related to the specific nature of the product and its synthesis pathway. In this study, we employed a continuous cultivation system to maintain defined source/sink conditions and metabolic states, allowing for a systematic and quantitative analysis of the effect of lactate production on photosynthetic and growth efficiency. This approach enables a realistic evaluation of the biotechnological potential of engineered cyanobacterial strains.
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
(2022)
Article
Biotechnology & Applied Microbiology
Lisa Bretschneider, Ingeborg Heuschkel, Katja Buehler, Rohan Karande, Bruno Buehler
Summary: This study successfully constructed a strain of Pseudomonas taiwanensis that efficiently converts cyclohexane to adipic acid, laying the foundation for environmentally friendly production of adipic acid and related polymers.
METABOLIC ENGINEERING
(2022)
Article
Biochemical Research Methods
Franz Opel, Nina A. Siebert, Sabine Klatt, Adrian Tuellinghoff, Janis G. Hantke, Joerg Toepel, Bruno Buehler, Dennis J. Nuernberg, Stephan Klaehn
Summary: Cyanobacteria have attracted great interest in biotechnology for their potential in sustainable, photosynthesis-driven production of fuels and value-added chemicals. However, compared to heterotrophic microorganisms, cyanobacterial model strains still lag behind in terms of molecular tools for engineering their metabolism. Researchers have developed a new tool called the pSOMA shuttle vector series for comprehensive genetic engineering of cyanobacteria and demonstrated its potential in gene expression and transfer.
ACS SYNTHETIC BIOLOGY
(2022)
Review
Biotechnology & Applied Microbiology
Eleni Theodosiou, Adrian Tuellinghoff, Jorg Toepel, Bruno Buehler
Summary: This review focuses on the development of efficient whole-cell biocatalysts and their connection with metabolic modules, cell growth, maintenance, and product formation. By redesigning and establishing metabolic modules, it is possible to maximize biosynthetic reactions and pathways, leading to high-yield, high-titer, and high-productivity industrial products.
FRONTIERS IN BIOENGINEERING AND BIOTECHNOLOGY
(2022)
Article
Agricultural Engineering
Jorg Toepel, Rohan Karande, Bruno Buehler, Katja Buehler, Andreas Schmid
Summary: Hydrogen (H2) is a promising fuel for climate neutral energy carriers, and photosynthesis-driven H2 production, which relies on sunlight and water, has shown potential. Research has been conducted using cyanobacteria as biocatalysts in capillary biofilm photobioreactors (CBRs). The study found that biofilm formation and stability are influenced by light and CO2 availability, and H2 production rates vary between different cyanobacteria species. By adjusting light and O2 levels, biofilm formation and H2 production could be enhanced, with high stability lasting for weeks. Final biocatalyst titers reached up to 100 g l-1, and H2 production rates were up to 300 mu mol H2 l-1h-1 and 3 mu mol H2 gcdw-1h-1 in biofilms.
BIORESOURCE TECHNOLOGY
(2023)
Article
Nanoscience & Nanotechnology
Rokas Garmasukis, Claudia Hackl, Christian Dusny, Christian Elsner, Ales Charvat, Andreas Schmid, Bernd Abel
Summary: This paper presents an innovative and low-cost method for rapid prototyping of microfluidic chips. The technique involves controlled deposition of aqueous microdroplets on a cooled surface to create printed ice microstructures, which are then coated with a UV-curable acrylic cover layer. The technology is applied to create a microfluidic chip for cell-customized optical-cell analysis, and the chip design is optimized for different cell types. The authors demonstrate the feasibility of using this chip for physiological analysis of different cell types.
MICROFLUIDICS AND NANOFLUIDICS
(2023)
Review
Biochemical Research Methods
Joerg Toepel, Rohan Karande, Stephan Klaehn, Bruno Buehler
Summary: Cyanobacteria have great potential to produce chemicals from sustainable resources through photosynthesis. Recent research on internal electron and carbon fluxes and their regulation provides new opportunities for efficient product formation. Novel photobioreactor concepts are being developed to ensure sufficient light supply. This review summarizes the latest developments in cyanobacterial engineering and highlights the importance of a holistic approach to establish photosynthesis-based production processes for a future green bioeconomy.
CURRENT OPINION IN BIOTECHNOLOGY
(2023)
Article
Biotechnology & Applied Microbiology
Adrian Tuellinghoff, Harcel Djaya-Mbissam, Joerg Toepel, Bruno Buehler
Summary: The photosynthetic light reaction in cyanobacteria was used to convert cyclohexanone into 6-hydroxyhexanoic acid. Co-expression of Baeyer-Villiger monooxygenase (BVMO) and lactonase from Acidovorax sp. CHX100 enabled the conversion with high activity and without inhibitory accumulation. This study demonstrates the feasibility of light-driven biocatalytic cascade operation in cyanobacteria.
PLANT BIOTECHNOLOGY JOURNAL
(2023)
Article
Biotechnology & Applied Microbiology
Carolin Bertelmann, Magdalena Mock, Andreas Schmid, Bruno Buehler
Summary: Steroid hydroxylations are important reactions in industry due to the pharmacological relevance of hydroxylated derivatives. However, these reactions suffer from low turnover rates, enzyme instability, and inhibition and toxicity. A new level of steroid hydroxylation rates has been achieved by introducing highly active CYP450 BM3 variants and the outer membrane protein AlkL. The activity tends to decrease, which may affect overall productivities. Poor testosterone solubility and inhibition by the main product were identified as causes of instability, and the instability of CYP450 BM3 variants is also a critical factor.
MICROBIAL BIOTECHNOLOGY
(2023)
Article
Microbiology
Mahir Bozan, Andreas Schmid, Katja Buehler
Summary: Cyanobacteria are promising microorganisms for sustainable photo-biotechnological production processes. In this study, different cyanobacteria were evaluated for their application in a novel capillary biofilm reactor, and Tolypothrix sp. PCC 7712 emerged as the best performer.
