Structural Elucidation of a Metagenomic Urethanase and Its Engineering Towards Enhanced Hydrolysis Profiles DOI Creative Commons
Thomas Bayer, Gottfried J. Palm, Leona Berndt

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(38)

Published: July 1, 2024

While plastics like polyethylene terephthalate can already be degraded efficiently by the activity of hydrolases, other synthetic polymers polyurethanes (PUs) and polyamides (PAs) largely resist biodegradation. In this study, we solved first crystal structure metagenomic urethanase UMG-SP-1, identified highly flexible loop regions to comprise active site residues, targeted a total 20 potential hot spots site-saturation mutagenesis. Engineering campaigns yielded variants with single mutations, exhibiting almost 3- 8-fold improved against stable N-aryl urethane amide bonds, respectively. Furthermore, demonstrated release corresponding monomers from thermoplastic polyester-PU PA (nylon 6) single, metagenome-derived after short incubation times. Thereby, expanded hydrolysis profile UMG-SP-1 beyond reported low-molecular weight carbamates. Together, these findings promise advanced strategies for bio-based degradation recycling plastic materials waste, aiding efforts establish circular economy polymers.

Language: Английский

Is enzyme immobilization a mature discipline? Some critical considerations to capitalize on the benefits of immobilization DOI Creative Commons
Juan M. Bolívar, John M. Woodley, Roberto Fernandéz‐Lafuente

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(15), P. 6251 - 6290

Published: Jan. 1, 2022

Enzyme immobilization has been developing since the 1960s and although many industrial biocatalytic processes use technology to improve enzyme performance, still today we are far from full exploitation of field. One clear reason is that evaluate based on only a few experiments not always well-designed. In contrast other reviews subject, here highlight pitfalls using incorrectly designed protocols explain why in cases sub-optimal results obtained. We also describe solutions overcome these challenges come conclusion recent developments material science, bioprocess engineering protein science continue open new opportunities for future. this way, immobilization, being mature discipline, remains as subject high interest where intense research necessary take advantage possibilities.

Language: Английский

Citations

355
From nature to industry: Harnessing enzymes for biocatalysis DOI
Rebecca Buller, Stefan Lutz, Romas J. Kazlauskas

et al.

Science, Journal Year: 2023, Volume and Issue: 382(6673)

Published: Nov. 23, 2023

Biocatalysis harnesses enzymes to make valuable products. This green technology is used in countless applications from bench scale industrial production and allows practitioners access complex organic molecules, often with fewer synthetic steps reduced waste. The last decade has seen an explosion the development of experimental computational tools tailor enzymatic properties, equipping enzyme engineers ability create biocatalysts that perform reactions not present nature. By using (chemo)-enzymatic synthesis routes or orchestrating intricate cascades, scientists can synthesize elaborate targets ranging DNA pharmaceuticals starch made vitro CO2-derived methanol. In addition, new chemistries have emerged through combination biocatalysis transition metal catalysis, photocatalysis, electrocatalysis. review highlights recent key developments, identifies current limitations, provides a future prospect for this rapidly developing technology.

Language: Английский

Citations

204
Hydrogen-bonded organic frameworks: design, applications, and prospects DOI Creative Commons

Lifang Chen,

Boying Zhang, Liling Chen

et al.

Materials Advances, Journal Year: 2022, Volume and Issue: 3(9), P. 3680 - 3708

Published: Jan. 1, 2022

Hydrogen-bonded organic frameworks (HOFs) are crystalline porous polymers which formed by the interaction of hydrogen bonding among building blocks. Unique advantages HOFs, enabling new platforms for exploring multifunctional applications.

Language: Английский

Citations

128
Biofuel production, hydrogen production and water remediation by photocatalysis, biocatalysis and electrocatalysis DOI Creative Commons
Ahmed I. Osman, Ahmed M. Elgarahy, Abdelazeem S. Eltaweil

et al.

Environmental Chemistry Letters, Journal Year: 2023, Volume and Issue: 21(3), P. 1315 - 1379

Published: March 10, 2023

Abstract The energy crisis and environmental pollution have recently fostered research on efficient methods such as catalysis to produce biofuel clean water. Environmental refers green catalysts used breakdown pollutants or chemicals without generating undesirable by-products. For example, derived from waste inexpensive materials are promising for the circular economy. Here we review photocatalysis, biocatalysis, electrocatalysis, with focus catalyst synthesis, structure, applications. Common include biomass-derived materials, metal–organic frameworks, non-noble metals nanoparticles, nanocomposites enzymes. Structure characterization is done by Brunauer–Emmett–Teller isotherm, thermogravimetry, X-ray diffraction photoelectron spectroscopy. We found that water can be degraded an efficiency ranging 71.7 100%, notably heterogeneous Fenton catalysis. Photocatalysis produced dihydrogen (H 2 ) generation rate higher than 100 μmol h −1 . Dihydrogen yields ranged 27 88% methane cracking. Biodiesel production reached 48.6 99%.

Language: Английский

Citations

113
Where Chemocatalysis Meets Biocatalysis: In Water DOI
Harald Gröger, Fabrice Gallou, Bruce H. Lipshutz

et al.

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(9), P. 5262 - 5296

Published: Dec. 6, 2022

Chemoenzymatic catalysis, by definition, involves the merging of sequential reactions using both chemocatalysis and biocatalysis, typically in a single reaction vessel. A major challenge, solution to which, however, is associated with numerous advantages, run such one-pot processes water: majority enzyme-catalyzed take place water as Nature's medium, thus enabling broad synthetic diversity when due option use virtually all types enzymes. Furthermore, cheap, abundantly available, environmentally friendly, making it, principle, an ideal medium. On other hand, most routinely performed today organic solvents (which might deactivate enzymes), appearing make it difficult combine biocatalysis toward cascades water. Several creative approaches solutions that enable combinations chemo- be realized applied problems are presented herein, reflecting state-of-the-art this blossoming field. Coverage has been sectioned into three parts, after introductory remarks: (1) Chapter 2 focuses on historical developments initiated area research; (2) 3 describes key post-initial discoveries have advanced field; (3) 4 highlights latest achievements provide attractive main question compatibility between (used predominantly aqueous media) (that remains solvents), Chapters covering mainly literature from ca. 2018 present. 5 6 brief overview where field stands, challenges lie ahead, ultimately, prognosis looking future chemoenzymatic catalysis synthesis.

Language: Английский

Citations

100
Mechanism-guided tunnel engineering to increase the efficiency of a flavin-dependent halogenase DOI
Kridsadakorn Prakinee, Aisaraphon Phintha,

Surawit Visitsatthawong

et al.

Nature Catalysis, Journal Year: 2022, Volume and Issue: 5(6), P. 534 - 544

Published: June 16, 2022

Language: Английский

Citations

86
Introducing Savie: A Biodegradable Surfactant Enabling Chemo- and Biocatalysis and Related Reactions in Recyclable Water DOI Creative Commons
Joseph R. A. Kincaid, Madison J. Wong, Nnamdi Akporji

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(7), P. 4266 - 4278

Published: Feb. 8, 2023

Savie is a biodegradable surfactant derived from vitamin E and polysarcosine (PSar) developed for use in organic synthesis recyclable water. This includes homogeneous catalysis (including examples employing only ppm levels of catalyst), heterogeneous catalysis, biocatalytic transformations, including multistep chemoenzymatic sequence. Use frequently leads to significantly higher yields than do conventional surfactants, while obviating the need waste-generating solvents.

Language: Английский

Citations

54
Photocatalyzed Enantioselective Functionalization of C(sp3)–H Bonds DOI
Guo‐Qiang Xu, Wei David Wang, Peng‐Fei Xu

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(2), P. 1209 - 1223

Published: Jan. 3, 2024

Owing to its diverse activation processes including single-electron transfer (SET) and hydrogen-atom (HAT), visible-light photocatalysis has emerged as a sustainable efficient platform for organic synthesis. These provide powerful avenue the direct functionalization of C(sp3)–H bonds under mild conditions. Over past decade, there have been remarkable advances in enantioselective bond via combined with conventional asymmetric catalysis. Herein, we summarize involving discuss two main pathways this emerging field: (a) SET-driven carbocation intermediates are followed by stereospecific nucleophile attacks; (b) photodriven alkyl radical further enantioselectively captured (i) chiral π-SOMOphile reagents, (ii) stereoselective transition-metal complexes, (iii) another distinct stereoscopic species. We aim key reaction design, catalyst development, mechanistic understanding, new insights into rapidly evolving area research.

Language: Английский

Citations

36
Recent advances in metal–organic frameworks for stimuli-responsive drug delivery DOI
Fei Xing, Jiawei Xu, Yuxi Zhou

et al.

Nanoscale, Journal Year: 2024, Volume and Issue: 16(9), P. 4434 - 4483

Published: Jan. 1, 2024

Metal-organic frameworks have become promising stimuli-responsive agents to release the loaded therapeutic in target site achieve more precise drug delivery due their high loading, excellent biocompatibility, and stimuli-responsiveness.

Language: Английский

Citations

30
Tailored Metal‐Organic Framework‐Based Nanozymes for Enhanced Enzyme‐Like Catalysis DOI Open Access
Zhichao Yu,

Zhenjin Xu,

Ruijin Zeng

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

Abstract The global crisis of bacterial infections is exacerbated by the escalating threat microbial antibiotic resistance. Nanozymes promise to provide ingenious solutions. Here, we reported a homogeneous catalytic structure Pt nanoclusters with finely tuned metal–organic framework (ZIF‐8) channel structures for treatment infected wounds. Catalytic site normalization showed that active aggregates fine‐tuned pore modifications had capacity 14.903×10 5 min −1 , which was 18.7 times higher than particles in monodisperse state ZIF‐8 (0.793×10 ). In situ tests revealed change from homocleavage heterocleavage hydrogen peroxide at interface nanozyme one key reasons improvement activity. Density‐functional theory and kinetic simulations reaction jointly determine role center substrate together. Metabolomics analysis developed nanozyme, working conjunction reactive oxygen species, could effectively block energy metabolic pathways within bacteria, leading spontaneous apoptosis rupture. This pioneering study elucidates new ideas regulation artificial enzyme activity provides perspectives development efficient substitutes.

Language: Английский

Citations

30