The E factor at 30: a passion for pollution prevention

Green Chemistry, Journal Year: 2023, Volume and Issue: 25(5), P. 1704 - 1728

Published: Jan. 1, 2023

Publication of the E Factor drew attention to problem waste in chemicals manufacture. Thirty yeas later it is abundantly clear that underlying cause global environmental problems, from climate change plastic pollution.

Language: Английский

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Concerted and Selective Electrooxidation of Polyethylene‐Terephthalate‐Derived Alcohol to Glycolic Acid at an Industry‐Level Current Density over a Pd−Ni(OH)₂ Catalyst

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(11)

Published: Jan. 19, 2023

Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H2 is an ideal solution to address severe plastic pollution. Here, we report the electrooxidation EG glycolic acid (GA) with a high Faraday efficiency selectivity (>85 %) even at industry-level current density (600 mA cm-2 1.15 V vs. RHE) over Pd-Ni(OH)2 catalyst. Notably, stable electrolysis 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental theoretical results reveal that 1) OH* generation promoted by Ni(OH)2 plays critical role in facilitating EG-to-GA oxidation removing poisonous carbonyl species, thereby achieving activity stability; 2) Pd downshifted d-band center oxophilic Ni synergistically facilitate rapid desorption transfer GA from active sites inactive sites, avoiding over-oxidation thus selectivity.

Language: Английский

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Expanding the Synthetic Toolbox through Metal–Enzyme Cascade Reactions

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(9), P. 5297 - 5346

Published: Jan. 10, 2023

The combination of metal-, photo-, enzyme-, and/or organocatalysis provides multiple synthetic solutions, especially when the creation chiral centers is involved. Historically, enzymes and transition metal species have been exploited simultaneously through dynamic kinetic resolutions racemates. However, more recently, linear cascades appeared as elegant solutions for preparation valuable organic molecules combining bioprocesses metal-catalyzed transformations. Many advantages are derived from this symbiosis, although there still bottlenecks to be addressed including successful coexistence both catalyst types, need compatible reaction media mild conditions, or minimization cross-reactivities. Therefore, here also provided by means coimmobilization, compartmentalization strategies, flow chemistry, etc. A comprehensive review presented focusing on period 2015 early 2022, which has divided into two main sections that comprise first use metals independent catalysts but working in an orchestral sequential manner, later their application bionanohybrid materials coimmobilization adequate supports. Each part classified different subheadings, based catalyzed catalyst, while development nonasymmetric stereoselective processes was considered section.

Language: Английский

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Single‐Atom Nanozymes for Catalytic Therapy: Recent Advances and Challenges

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(16)

Published: Jan. 4, 2024

Abstract As a powerful tool, nanozyme catalysts broaden the avenues to implement bio‐inspired solutions for addressing many important concerns, covering energy, healthcare, environment, and more. Recent endeavors, characterized by atomic precision, have enabled extensive exploration of single‐atom nanozymes (SAzymes) with high catalytic activity, superior substrate selectivity, integrated multifunctionalities, thus becoming an emerging field that bridges nanotechnology biology. This review provides brief outline progress summarizes latest research advances regarding SAzymes in biomedical therapeutics, mainly including tumor therapy, wound antibacterial tissue anti‐inflammatory focus on their prototypical synthesis therapeutic mechanisms. Finally, current challenges future perspectives engineering advanced are also discussed outlooked. It is anticipated this area shall provide useful guidance therapy.

Language: Английский

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Exploring Emergent Properties in Enzymatic Reaction Networks: Design and Control of Dynamic Functional Systems

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(5), P. 2553 - 2582

Published: March 4, 2024

The intricate and complex features of enzymatic reaction networks (ERNs) play a key role in the emergence sustenance life. Constructing such vitro enables stepwise build up complexity introduces opportunity to control activity using physicochemical stimuli. Rational design modulation network motifs enable engineering artificial systems with emergent functionalities. Such functional are useful for variety reasons as creating new-to-nature dynamic materials, producing value-added chemicals, constructing metabolic modules synthetic cells, even enabling molecular computation. In this review, we offer insights into chemical characteristics ERNs while also delving their potential applications associated challenges.

Language: Английский

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Navigating the landscape of enzyme design: from molecular simulations to machine learning

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(16), P. 8202 - 8239

Published: Jan. 1, 2024

Global environmental issues and sustainable development call for new technologies fine chemical synthesis waste valorization. Biocatalysis has attracted great attention as the alternative to traditional organic synthesis. However, it is challenging navigate vast sequence space identify those proteins with admirable biocatalytic functions. The recent of deep-learning based structure prediction methods such AlphaFold2 reinforced by different computational simulations or multiscale calculations largely expanded 3D databases enabled structure-based design. While approaches shed light on site-specific enzyme engineering, they are not suitable large-scale screening potential biocatalysts. Effective utilization big data using machine learning techniques opens up a era accelerated predictions. Here, we review applications machine-learning guided We also provide our view challenges perspectives effectively employing design integrating molecular learning, importance database construction algorithm in attaining predictive ML models explore fitness landscape

Language: Английский

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Rational multienzyme architecture design with iMARS

Cell, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Biocatalytic cascades with spatial proximity can orchestrate multistep pathways to form metabolic highways, which enhance the overall catalytic efficiency. However, effect of organization on activity is poorly understood, and multienzyme architectural engineering predictable performance remains unrealized. Here, we developed a standardized framework, called iMARS, rapidly design optimal architecture by integrating high-throughput tests structural analysis. The approach showed potential for industrial-scale applications, artificial fusion enzymes designed iMARS significantly improving production resveratrol 45.1-fold raspberry ketone 11.3-fold in vivo, as well enhancing ergothioneine synthesis fed-batch fermentation. In addition, greatly enhanced vitro efficiency complexes PET plastic depolymerization vanillin biosynthesis. As generalizable flexible strategy at molecular level, could facilitate green chemistry, synthetic biology, biomanufacturing.

Language: Английский

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Putting precision and elegance in enzyme immobilisation with bio-orthogonal chemistry

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(16), P. 7281 - 7304

Published: Jan. 1, 2022

The covalent immobilisation of enzymes generally involves the use highly reactive crosslinkers, such as glutaraldehyde, to couple enzyme molecules each other or carriers through, for example, free amino groups lysine residues, on surface. Unfortunately, methods suffer from a lack precision. Random formation linkages with functional in leads disruption three dimensional structure and accompanying activity losses. This review focuses recent advances bio-orthogonal chemistry conjunction rec-DNA affect precise enzymes. In this way, cost-effective combination production, purification an is achieved, single unit operation high degree Various techniques putting precision elegance into are elaborated. These include, fusing (grafting) peptide protein tags target that enable its cell lysate incorporating non-standard acids application chemistry.

Language: Английский

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Chemoenzymatic Cascades Combining Biocatalysis and Transition Metal Catalysis for Asymmetric Synthesis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(18)

Published: Feb. 6, 2023

Abstract The combination of catalytic methods provides multiple advantages in organic synthesis, allowing access to diverse molecules a straightforward manner. Merging metal and enzyme catalysis is currently receiving great attention due the possibility assemble C−C coupling, olefin metathesis, hydration other reactions with exquisite stereospecificity displayed by enzymes. Thus, this minireview organized based on action species (Pd, Ru, Au, Ir, Fe…) different Special will be paid design sequential processes concurrent cascades, presenting solutions such as use surfactants or compartmentalization strategies for those cases where incompatibilities could hamper overall process.

Language: Английский

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Strategies for Improving Transdermal Administration: New Approaches to Controlled Drug Release

Pharmaceutics, Journal Year: 2023, Volume and Issue: 15(4), P. 1183 - 1183

Published: April 7, 2023

In this work, we aim to address several strategies improve transdermal drug delivery, such as iontophoresis, sonophoresis, electroporation and micron. We also propose a review of some patches their applications in medicine. TDDs (transdermal with delayed active substances) are multilayered pharmaceutical preparations that may contain one or more substances, which, systemic absorption is achieved through intact skin. The paper presents new approaches the controlled release drugs: niosomes, microemulsions, transfersomes, ethosomes, but hybrid nanoemulsions microns. novelty lies presentation administration drugs, combined medicine, light technological developments.

Language: Английский

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