Chemical Science, Год журнала: 2022, Номер 13(10), С. 2809 - 2823
Опубликована: Янв. 1, 2022
This perspective highlights the growing body of literature that leverages polarity reversal (umpolung reactivity) for selective modification proteinogenic functionalities and identifies opportunities further innovation.
Язык: Английский
Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 5225 - 5261
Опубликована: Янв. 20, 2023
Because sunlight is the most abundant energy source on earth, it has huge potential for practical applications ranging from sustainable supply to light driven chemistry. From a chemical perspective, excited states generated by make thermodynamically uphill reactions possible, which forms basis storage into fuels. In addition, with light, open-shell species can be open up new reaction pathways in organic synthesis. Crucial are photosensitizers, absorb and transfer substrates various mechanisms, processes that highly depend distance between molecules involved. Supramolecular coordination cages well studied synthetically accessible vessels single cavities guest binding, ensuring close proximity of different components. Due high modularity their size, shape, nature metal centers ligands, ideal platforms exploit preorganization photocatalysis. Herein we focus application supramolecular photocatalysis artificial photosynthesis photo(redox) catalysis. Finally, brief overview immobilization strategies provides tools implementing devices. This review inspiration future design photocatalytic host-guest systems producing solar fuels complex molecules.
Язык: Английский
Процитировано
171
Journal of the American Chemical Society, Год журнала: 2023, Номер 145(6), С. 3535 - 3542
Опубликована: Фев. 2, 2023
Homogeneous organic photocatalysis typically requires molecular photosensitizers absorbing in the ultraviolet-visible (UV/vis) region, because UV/vis photons possess sufficient energy to excite those one-photon-absorbing desired excited states. However, light irradiation has many potential limitations, especially for large-scale applications, such as low penetration through reaction media, competing absorption by substrates and co-catalysts, incompatibility with bearing light-sensitive functionalities. In fact, these drawbacks can be effectively avoided if near infrared (NIR) utilized drive target reactions. Herein, we report two benzothiazole-derived compounds novel two-photon-absorbing (TPA) photosensitizers, which function under NIR using inexpensive LED source. We demonstrate that judicially modulating donor-π-acceptor-π-donor-conjugated structure containing a bibenzothiazole core imine bridges, excellent two-photon capability region achieved, approaching 2000 GM at 850 nm. Together large quantum yields (∼0.5), TPA exhibit performance driving various O2-involved reactions upon nm, showing great depth, superior blue irradiation. A suite of photophysical computational studies were performed shed on underlying electronic states responsible observed capability. Overall, this work highlights promise developing Ru/Ir-free operative taking advantage mechanism.
Язык: Английский
Процитировано
73
Nature, Год журнала: 2023, Номер 621(7980), С. 753 - 759
Опубликована: Авг. 23, 2023
Privileged chiral catalysts-those that share common structural features and are enantioselective across a range of reactions-continue to transform the chemical-research landscape1. In recent years, new reactivity modes have been achieved through excited-state catalysis, processes activated by light, but it is unclear if selectivity ground-state privileged catalysts can be matched. Although interception photogenerated intermediates cycles has partially addressed this challenge2, single, photocatalysts simultaneously regulate conspicuously scarce3. So far, precision donor-acceptor recognition motifs remain crucial in photocatalyst design4. Here we show Al-salen complexes, which well-defined photophysical properties, used for efficient photochemical deracemization5 cyclopropyl ketones (up 98:2 enantiomeric ratio (e.r.)). Irradiation at λ = 400 nm (violet light) augments commercial catalyst enable enantioselectivity regulated simultaneously. This circumvents need tailored catalyst-substrate motifs. It predicted study will stimulate re-evaluation many venerable (ground-state) processes, ultimately leading identification candidates may considered 'privileged' both models.
Язык: Английский
Процитировано
66
Chemical Reviews, Год журнала: 2023, Номер 123(16), С. 9720 - 9785
Опубликована: Июль 17, 2023
Endogenous photosensitizers play a critical role in both beneficial and harmful light-induced transformations biological systems. Understanding their mode of action is essential for advancing fields such as photomedicine, photoredox catalysis, environmental science, the development sun care products. This review offers comprehensive analysis endogenous human skin, investigating connections between electronic excitation subsequent activation or damage organic biomolecules. We gather physicochemical photochemical properties key examine relationships chemical reactivity, location within primary biochemical events following solar radiation exposure, along with influence on skin physiology pathology. An important take-home message this that photosensitization allows visible light UV-A to have large effects skin. The presented here unveils potential causes continuous increase global cancer cases emphasizes limitations current protection approaches.
Язык: Английский
Процитировано
50
Chemical Reviews, Год журнала: 2023, Номер 123(24), С. 14038 - 14083
Опубликована: Ноя. 2, 2023
Incorporating sulfur (S) atoms into polymer main chains endows these materials with many attractive features, including a high refractive index, mechanical properties, electrochemical and adhesive ability to heavy metal ions. The copolymerization involving S-containing monomers constitutes facile method for effectively constructing polymers diverse structures, readily tunable sequences, topological structures. In this review, we describe the recent advances in synthesis of via or multicomponent polymerization techniques concerning variety monomers, such as dithiols, carbon disulfide, carbonyl sulfide, cyclic thioanhydrides, episulfides elemental (S8). Particularly, significant focus is paid precise control main-chain sequence, stereochemistry, structure achieving high-value applications.
Язык: Английский
Процитировано
49
Nature Reviews Chemistry, Год журнала: 2024, Номер 8(4), С. 238 - 255
Опубликована: Март 21, 2024
Язык: Английский
Процитировано
35
Journal of the American Chemical Society, Год журнала: 2025, Номер unknown
Опубликована: Фев. 28, 2025
The advent of bioorthogonal chemistry has transformed scientific research, offering a powerful tool for selective and noninvasive labeling (bio)molecules within complex biological environments. This innovative approach facilitated the study intricate cellular processes, protein dynamics, interactions. Nevertheless, number challenges remain to be addressed, including need improved reaction kinetics, enhanced biocompatibility, development more diverse orthogonal set reactions. While scientists continue search veritable solutions, remains transformative with vast potential advancing our understanding biology medicine. Perspective offers insights into reactions commonly classified as "bioorthogonal", which, however, may not always demonstrate desired selectivity regarding interactions between their components additives or catalysts used under conditions.
Язык: Английский
Процитировано
4
Organic & Biomolecular Chemistry, Год журнала: 2025, Номер unknown
Опубликована: Янв. 1, 2025
This review provides an account of the tryptophan-specific conjugation peptides and proteins its extensive application in imaging living cells, radiolabelling proteins, protein engineering, etc .
Язык: Английский
Процитировано
3
Chemistry - A European Journal, Год журнала: 2021, Номер 28(18)
Опубликована: Дек. 29, 2021
Inspired by human vision, a diverse range of light-driven molecular switches and motors have been developed for fundamental understanding application in material science biology. Recently, the design synthesis visible actively pursued. This emerging trend is partly motivated to avoid harmful effects ultraviolet light, which was necessary drive classical at least one direction, impeding their employment biomedical photopharmacology applications. Moreover, are demonstrated enable benign optical materials advanced photonic devices. Therefore, during past several years, based on azobenzene derivatives, diarylethenes, 1,2-dicyanodithienylethenes, hemithioindigo iminothioindoxyls, donor-acceptor Stenhouse adducts, overcrowded alkene judiciously designed, synthesized, used development functional systems wide In this Review, we present recent developments toward motors, with applications fabrication science, bioscience, pharmacology, etc. The realized so far undoubtedly widen scope these interesting compounds technological biological We hope Review article could provide additional impetus inspire further research interests future exploration materials, systems,
Язык: Английский
Процитировано
95
Journal of the American Chemical Society, Год журнала: 2021, Номер 144(1), С. 23 - 41
Опубликована: Дек. 30, 2021
Although electrochemical strategies for small-molecule synthesis are flourishing, this technology has yet to be fully exploited the mild and chemoselective modification of peptides proteins. With growing number diverse peptide natural products being identified emergence modified proteins as therapeutic diagnostic agents, methods stand alluring prospects harnessing reactivity polypeptides build molecular complexity. As a inherently tunable reaction platform, electrochemistry is arguably well-suited overcome chemo- regioselectivity issues which limit existing bioconjugation strategies. This Perspective will showcase recently developed approaches protein modification. The article also highlights wealth untapped opportunities production homogeneously biomolecules, with an eye toward realizing enormous potential chemistry.
Язык: Английский
Процитировано
85