Fine‐Tuning of Chiral Microenvironments within Triple‐Stranded Helicates for Enhanced Enantioselectivity DOI
Jingjing Jiao, Jinqiao Dong, Yingguo Li

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(30), P. 16568 - 16575

Published: May 3, 2021

Abstract Here we report the formation of an unexpected and unique family chiral helicates. Crystal structures show that these triple‐stranded Zn II 2 L 3 complexes are held together by subcomponent assembly axially diamine‐functionalized 1,1′‐biphenol ditopic with 2‐formylpyridine . Specifically, molecular helicity can be controlled absolute configurations bimetallic vertices, which has been shown to homoconfiguration (ΔΔ) or mesomeric configuration (ΔΛ), depending critically on bulky groups length spacers. Fascinatingly, in this system engineer space‐restricted microenvironments varied polar apolar moieties, profoundly influence binding affinities discrimination properties helicates, leading highly enantio‐ helix‐sense‐selective recognition for amino alcohols (up 9.35). This work reveals transformation single‐molecule chirality global supramolecular within well‐defined helicates demonstrates their dependent superior microenvironments.

Language: Английский

A Global Review on Short Peptides: Frontiers and Perspectives DOI Creative Commons
Vasso Apostolopoulos, Joanna Bojarska, Tsun‐Thai Chai

et al.

Molecules, Journal Year: 2021, Volume and Issue: 26(2), P. 430 - 430

Published: Jan. 15, 2021

Peptides are fragments of proteins that carry out biological functions. They act as signaling entities via all domains life and interfere with protein-protein interactions, which indispensable in bio-processes. Short peptides include fundamental molecular information for a prelude to the symphony life. have aroused considerable interest due their unique features great promise innovative bio-therapies. This work focusing on current state-of-the-art short peptide-based therapeutical developments is first global review written by researchers from continents, celebration 100 years peptide therapeutics since commencement insulin therapy 1920s. Peptide “drugs” initially played only role hormone analogs balance disorders. Nowadays, they achieve numerous biomedical tasks, can cross membranes, or reach intracellular targets. The bio-processes hardly be mimicked other chemical substances. article divided into independent sections, related either progress theranostics problems posing challenge bio-medicine. In particular, SWOT analysis peptides, relevance therapies diverse diseases, improvements (bio)synthesis platforms, advanced nano-supramolecular technologies, aptamers, altered ligands silico methodologies overcome limitations, modern smart bio-functional materials, vaccines, drug/gene-targeted delivery systems discussed.

Language: Английский

Citations

310

Nonenzymatic Metabolic Reactions and Life’s Origins DOI
Kamila B. Muchowska, Sreejith J. Varma, Joseph Moran

et al.

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(15), P. 7708 - 7744

Published: July 20, 2020

Prebiotic chemistry aims to explain how the biochemistry of life as we know it came be. Most efforts in this area have focused on provisioning compounds importance by multistep synthetic routes that do not resemble biochemistry. However, gaining insight into why core metabolism uses molecules, reactions, pathways, and overall organization does requires us consider molecules only end goals. Equally important are dynamic processes build them up break down. This perspective has led many researchers hypothesis first stage origin began with onset a primitive nonenzymatic version metabolism, initially catalyzed naturally occurring minerals metal ions. view life's origins come be known "metabolism first". Continuity modern would require down ketoacids, sugars, amino acids, ribonucleotides much same way pathways today. review discusses metabolic relevance manner accessible chemists, summarizes experiments suggesting several might their roots prebiotic chemistry. Finally, key remaining milestones for protometabolic highlighted.

Language: Английский

Citations

267

Chemically Fueled Self‐Assembly in Biology and Chemistry DOI Creative Commons
Krishnendu Das, Luca Gabrielli, Leonard J. Prins

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(37), P. 20120 - 20143

Published: March 11, 2021

Life is a non-equilibrium state of matter maintained at the expense energy. Nature uses predominantly chemical energy stored in thermodynamically activated, but kinetically stable, molecules. These high-energy molecules are exploited for synthesis other biomolecules, activation biological machinery such as pumps and motors, maintenance structural order. Knowledge how transferred to biochemical processes essential development artificial systems with life-like processes. Here, we discuss can be used control organization organic Four different strategies have been identified according distinguishable physical-organic basis. For each class, one example from biology chemistry discussed detail illustrate practical implementation concept distinct opportunities they offer. Specific attention paid discussion chemically fueled self-assembly. We meaning self-assembly, its kinetic origin, develop synthetic systems.

Language: Английский

Citations

264

Recent progress in non-native nucleic acid modifications DOI
Luke K. McKenzie, Roberto El-Khoury,

James D. Thorpe

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 5126 - 5164

Published: Jan. 1, 2021

While Nature harnesses RNA and DNA to store, read write genetic information, the inherent programmability, synthetic accessibility wide functionality of these nucleic acids make them attractive tools for use in a vast array applications.

Language: Английский

Citations

222

Mechanochemistry: New Tools to Navigate the Uncharted Territory of “Impossible” Reactions DOI Creative Commons
Federico Cuccu, Lidia De Luca, Francesco Delogu

et al.

ChemSusChem, Journal Year: 2022, Volume and Issue: 15(17)

Published: July 21, 2022

Mechanochemical transformations have made chemists enter unknown territories, forcing a different chemistry perspective. While questioning or revisiting familiar concepts belonging to solution chemistry, mechanochemistry has broken new ground, especially in the panorama of organic synthesis. Not only does it foster "thinking outside box", but also opened reaction paths, allowing overcome weaknesses traditional exactly where use well-established solution-based methodologies rules out progress. In this Review, reader is introduced an intriguing research subject not yet fully explored and waiting for improved understanding. Indeed, study mainly focused on that, although impossible solution, become possible under mechanochemical processing conditions, simultaneously entailing innovation expanding chemical space.

Language: Английский

Citations

193

Spontaneous Deracemizations DOI
Thomas Buhse, José‐Manuel Cruz, María E. Noble‐Terán

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(4), P. 2147 - 2229

Published: Jan. 19, 2021

Spontaneous deracemizations is a challenging, multidisciplinary subject in current chirality research. In the absence of any chiral inductors, an achiral substance or racemic composition driven into enantioenriched even homochiral state through selective energy input, e.g., chemical potential, photoirradiation, mechanical grinding, ultrasound waves, thermal gradients, etc. The most prominent examples such transformations are Soai reaction and Viedma deracemization. this review, we track recent developments topic recall that many other have been reported for solutions from mesophases to conglomerate crystallizations. A compiled set simply available organic, inorganic, organometallic, MOF compounds, yielding crystals, should give impetus realize new experiments on spontaneous deracemizations. Taking account thermodynamic constraints, modeling efforts shown structural features alone not sufficient describe As guideline particular attention paid physicochemical origin symmetry requirements processes.

Language: Английский

Citations

147

Synthetic connectivity, emergence, and self-regeneration in the network of prebiotic chemistry DOI
Agnieszka Wołos, Rafał Roszak, Anna Żądło‐Dobrowolska

et al.

Science, Journal Year: 2020, Volume and Issue: 369(6511)

Published: Sept. 25, 2020

The challenge of prebiotic chemistry is to trace the syntheses life's key building blocks from a handful primordial substrates. Here we report forward-synthesis algorithm that generates full network chemical reactions accessible these substrates under generally accepted conditions. This contains both reported and previously unidentified routes biotic targets, as well plausible abiotic molecules. It also exhibits three forms nontrivial emergence, molecules within can act catalysts downstream reaction types; form functional systems, including self-regenerating cycles; produce surfactants relevant primitive biological compartmentalization. To support claims, computer-predicted, several multistep, self-regenerative cycle iminodiacetic acid were validated by experiment.

Language: Английский

Citations

146

Possible chemical and physical scenarios towards biological homochirality DOI Creative Commons
Quentin Sallembien, Laurent Bouteiller, Jeanne Crassous

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(9), P. 3436 - 3476

Published: Jan. 1, 2022

The single chirality of biological molecules in terrestrial biology raises more questions than certitudes about its origin. emergence homochirality (BH) and connection with the appearance life have elicited a large number theories related to generation, amplification preservation chiral bias under prebiotically relevant conditions. However, global scenario is still lacking. Here, possibility inducing significant "from scratch", i.e. absence pre-existing enantiomerically-enriched chemical species, will be considered first. It includes phenomena that are inherent nature matter itself, such as infinitesimal energy difference between enantiomers result violation parity certain fundamental interactions, physicochemical processes interactions organic physical fields, polarized particles, spins surfaces. spontaneous detectable sources has recently undergone advances thanks deracemization conglomerates through Viedma ripening asymmetric auto-catalysis Soai reaction. All these commonly discussed plausible asymmetry prebiotic conditions potentially accountable for primeval life. Then, several scenarios aimed reflect different debates BH: extra-terrestrial or origin (where?), mechanisms leading propagation enhancement (how?) temporal sequence homochirality, BH (when?). Intense ongoing regarding optically pure at moments evolution process towards life, levels building blocks Life, instructed functional polymers, even later stage elaborated systems, critically discussed. underlying principles experimental evidence commented each particular attention on those induction enantiomeric excesses proteinogenic amino acids, natural sugars, their intermediates derivatives. aim this review propose an updated timely synopsis order stimulate new efforts interdisciplinary field.

Language: Английский

Citations

115

Perspectives on recent advancements in energy harvesting, sensing and bio-medical applications of piezoelectric gels DOI Creative Commons
Thangavel Vijayakanth, Sudha Shankar, Gal Finkelstein-Zuta

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6191 - 6220

Published: Jan. 1, 2023

This review highlights the recent progress in piezoelectric gels (also known as PiezoGels) comprised of polymers, ceramic oxides and supramolecular materials used for energy harvesting, sensing wound dressing.

Language: Английский

Citations

70

Dipeptide coacervates as artificial membraneless organelles for bioorthogonal catalysis DOI Creative Commons
Shoupeng Cao, Tsvetomir Ivanov,

Julian Heuer

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Jan. 2, 2024

Abstract Artificial organelles can manipulate cellular functions and introduce non-biological processes into cells. Coacervate droplets have emerged as a close analog of membraneless organelles. Their biomimetic properties, such molecular crowding selective partitioning, make them promising components for designing cell-like materials. However, their use artificial has been limited by complex structure, control over internal microenvironment inherent colloidal instability. Here we report the design dipeptide coacervates that exhibit enhanced stability, biocompatibility, hydrophobic microenvironment. The character facilitates encapsulation species, including transition metal-based catalysts, enhancing efficiency in aqueous environments. Dipeptide carrying catalyst are incorporated active cells trigger an chemical reaction. development with opens alternative avenue field materials applications catalysis synthetic biology.

Language: Английский

Citations

55