Co‐compartmentalization of Enzymes and Cofactors within Pickering Emulsion Droplets for Continuous‐Flow Catalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(45)

Published: Sept. 16, 2022

Co-immobilization of enzymes and cofactors in a manner suitable for use continuous flow catalysis remains great challenge because the difficulty ensuring free accessibility immobilized cofactors. Herein, we present system based on co-compartmentalization within Pickering emulsion droplets, enabling regeneration droplets. As exemplified by enzyme-catalyzed ketone enantioselective reduction transamination, our systems exhibit long-term stability (300-400 h), outstanding total turnover number (TTN, 59204 mol mol-1 ) several-fold enhancement enzyme catalytic efficiency (CEe comparison to conventional biphasic reactions. well as giving insight into effects, will provide opportunity significantly advance continuous-flow biocatalysis towards level practical applications.

Language: Английский

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Non-canonical amino acids as a tool for the thermal stabilization of enzymes

Protein Engineering Design and Selection, Journal Year: 2023, Volume and Issue: 36

Published: Jan. 1, 2023

Abstract Biocatalysis has become a powerful alternative for green chemistry. Expanding the range of amino acids used in protein biosynthesis can improve industrially appealing properties such as enantioselectivity, activity and stability. This review will specifically delve into thermal stability improvements that non-canonical (ncAAs) confer to enzymes. Methods achieve this end, use halogenated ncAAs, selective immobilization rational design, be discussed. Additionally, specific enzyme design considerations using ncAAs are discussed along with benefits limitations various approaches available enhance

Language: Английский

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p-Xylene Oxidation to Terephthalic Acid: New Trends

Molecules, Journal Year: 2023, Volume and Issue: 28(4), P. 1922 - 1922

Published: Feb. 17, 2023

Large-scale terephthalic acid production from the oxidation of p-xylene is an especially important process in polyester industry, as it mainly used polyethylene terephthalate (PET) manufacturing, a polymer that widely fibers, films, and plastic products. This review presents discusses catalytic advances new trends (since 2014), innovations purification processes, simulations reactors reaction mechanisms.

Language: Английский

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Enzymatic Oxy‐ and Amino‐Functionalization in Biocatalytic Cascade Synthesis: Recent Advances and Future Perspectives

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(48)

Published: Aug. 28, 2023

Biocatalytic cascades are a powerful tool for building complex molecules containing oxygen and nitrogen functionalities. Moreover, the combination of multiple enzymes in one pot offers possibility to minimize downstream processing waste production. In this review, we illustrate various recent efforts development multi-step syntheses involving C-O C-N bond-forming produce high value-added compounds, such as pharmaceuticals polymer precursors. Both vitro vivo examples discussed, revealing respective advantages drawbacks. The use engineered boost outcome is also addressed current co-substrate cofactor recycling strategies presented, highlighting importance atom economy. Finally, tools overcome challenges multi-enzymatic oxy- amino-functionalization reactions including flow systems with immobilized biocatalysts confined nanomaterials.

Language: Английский

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Direct Z-Scheme Polymer/Polymer Double-Shell Hollow Nanostructures for Efficient NADH Regeneration and Biocatalytic Artificial Photosynthesis under Visible Light

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4433 - 4443

Published: March 17, 2023

The design of a highly efficient polymer photocatalyst is an essential prerequisite for photo-biocatalysis in polymer–enzyme coupled system, which offers important platform the synthesis pharmaceuticals and fine chemicals. However, current polymers still suffer drawbacks poor water wettability, low visible light absorption, high recombination rate photoinduced electron/hole pairs, severely limit their application photo-biocatalysis. Herein, we demonstrate polymer/polymer double-shell hollow nanostructure (PCN@PDBTS-HN) via facile two-step polymerization with polymeric carbon nitride (PCN) poly-dibenzothiophene sulfone (PDBTS) as internal external shells, respectively. covalent connection those two layers ensures spontaneous electron transfer from PDBTS to PCN, reflected X-ray photoelectron spectroscopy (XPS), paramagnetic resonance (EPR), fluorescence spectra, could effectively accelerate charge separation migration. Thanks its improved light-harvesting, increased hydrophilicity, enhanced redox capacity, obtained PCN@PDBTS-HN demonstrates excellent catalytic efficiency visible-light-promoted NADH regeneration conversion 85.4% being achieved 40 min (turnover frequency 0.859 mmol g–1 h–1). This value 1.4 2.6 times higher than that pristine PCN PDBTS, respectively, indicating role Z-scheme heterojunction improving efficiency. In addition, also displays photocatalytic selectivity 1,4-NADH regeneration, remarkable photostability, good biocompatibility. A total amount 2.12 mM methanol 8.39 l-glutamate was accumulated polymer/alcohol dehydrogenase (YADH) polymer/glutamate (GDH) implying flexibility chemical production photo-biocatalytic approach.

Language: Английский

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