Macromolecular Rapid Communications, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 13, 2024
A photo-assisted process is explored for improving the synthesis of oligo(triazole amide)s, which are prepared by solid phase using a repeated cycle two reactions: amine-carboxylic acid coupling and copper-catalyzed azide-alkyne cycloaddition (CuAAC). The improvement second reaction investigated herein. catalytic system involving Cu(II)Cl
Language: Английский
Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 523, P. 216247 - 216247
Published: Oct. 7, 2024
Language: Английский
Citations
1
Macromolecular Rapid Communications, Journal Year: 2024, Volume and Issue: 45(22)
Published: Aug. 6, 2024
Abstract Digitally‐encoded poly(phosphodiesters) ( d ‐PPDE) with highly complex primary structures are evaluated for layer‐by‐layer (LbL) assembly. To be easily decoded by mass spectrometry (MS), these digital polymers contain many different monomers: 2 coding units allowing binary encryption, 1 cleavable spacer controlled MS fragmentation, and 3 tags fragment identification. These heteropolymers therefore composed of 6 motifs. Despite this strong sequence heterogeneity, it is found that they enable a LbL film formation. For instance, regular growth observed when alternating the deposition negatively‐charged ‐PPDE positively‐charged poly(allyl amine hydrochloride) (PAH). Yet, in approach, interdistance between consecutive coded layers remains relatively small, which may an issue data storage applications, especially selective decoding stored information. Using poly(sodium 4‐styrene sulfonate) (PSS) as intermediate non‐coded polyanion, shown can achieved, while still maintaining growth. Last but not least, work small molecular weight (i.e., significantly smaller than those PAH PSS) enables
Language: Английский
Citations
1
Chemical Science, Journal Year: 2024, Volume and Issue: 15(36), P. 14938 - 14945
Published: Jan. 1, 2024
The need for reliable information storage is on a steep rise. Sequence-defined polymers, particularly oligonucleotides, are already in use several areas, while compound mixtures also offer simple way storing information. We investigated the of set isotopologues by mixing, where stored form mass spectrometric (MS) fingerprint mixture. A small molecule with 24 non-labile and replaceable hydrogen atoms was selected as model, components covering D
Language: Английский
Citations
1
Macromolecules, Journal Year: 2024, Volume and Issue: 57(21), P. 10454 - 10462
Published: Oct. 23, 2024
Coil–globule transition in a single-chain polymer is the cornerstone of physics. Although completely understood for homopolymers, it turns out to be much more sophisticated copolymers mere two nonionic monomers because position and especially sharpness (cooperativity) conformational change them are highly sequence-dependent. In this work, statistical theory coil–globule neutral AB with regular sequences developed. To describe role primary structure, we go beyond mean-field approximation calculate Gaussian fluctuation correction due chemical differences (incompatibility) between A B monomers. Local compositional fluctuations reduce second third virial coefficients monomer interactions; these corrections found general form, closed-form expressions provided block-alternating chains block length m. For nonperiodic sequences, annealed averages. Increasing blockiness shown (i) make globule denser, (ii) shift higher temperatures, and, most importantly, (iii) narrow region. The collapse sharpens strongly when accompanied or shortly followed by intraglobular microphase separation. developed contributes comprehensive understanding sequence-tunable behavior macromolecules, including Khokhlov–Khalatur protein-like forming globules core–shell microstructure.
Language: Английский
Citations
1
Soft Matter, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
Six different flexible stereocontrolled oligo(triazole-urethane)s substituted by precise sequences of nucleobases or analogs are synthesized. Molecular dynamics simulations indicate that the flexibility backbone leads to unspecific complexation pairs oligomers, irrespective complementarity their sequences. This is ascribed existence other interactions between as well spatial blurring sequence order encoded in chemical structure chain due its flexibility. The same conclusions drawn when investigating irreversible adsorption probe oligomers onto a layer target grafted click chemistry mushroom configuration on silicon substrate. In contrast, denser brush configurations, becomes more specific, with it being twice probable chains complementary would be irreversibly-bound than those non-complementary sequence. lateral excluded volume brush, leading partial stretching and increased preservation information contained monomer chains. At even higher grafting densities, however, penetration increasingly difficult, resulting loss binding efficiency. Our work thus demonstrates adverse role specificity nucleobase-functionalized provides directions for an improvement tuning density
Language: Английский
Citations
0
Elsevier eBooks, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
Citations
0
Macromolecular Chemistry and Physics, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 15, 2024
Abstract This study presents the exploration of sequence‐defined polyurethanes (PUs) as a new class heteropolymers capable precise conformational control. Utilizing molecular dynamics simulations, folding behavior polyurethane chains is investigated varying lengths (11, 20, and 50 monomers) in both vacuum aqueous environments. The simulations reveal that heterogeneous systematically refold to approach designed target structures better than non‐designed or with artificially disrupted hydrogen‐bond networks. subsequent synthesis an optimized 11‐mer sequence (P1) achieved through solid‐phase chemistry, thorough characterization via NMR, MS, SEC confirming accuracy predicted its controlled chain length. Solubility tests showed favorable results across multiple solvents, highlighting versatility polymer. research underscores potential emulate structural functional attributes biological macromolecules, opening pathways for their application catalysis, drug delivery, advanced material design. findings illustrate promising direction development synthetic polymers tailored properties, emphasizing transformative impact control polymer chemistry.
Language: Английский
Citations
0
Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 16, 2024
Abstract The selective monoaddition of polymerizable vinyl monomers like styrenes and methacrylates in a living manner has been achieved for the flash‐flow preparation molecules defined sequence with high selectivity. We demonstrated sequence‐defined synthesis multifunctional using an initiator, functionalized styrenes, diarylethylenes, various methacrylates, electrophilic trapping reagent at terminus (six‐component sequential connection maximum) without any intermediate purification steps. anionic flow system described herein is active polymerization, such that styrene or methacrylate can be expanded to afford highly dispersed oligomers affecting other single units, which means unequivocal sequences were successfully inserted into internal terminal positions. methodology provides adaptable method construction new molecular spaces based on unimolecular control pinpoint functionalization.
Language: Английский
Citations
0
ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(43), P. 58973 - 58979
Published: Oct. 18, 2024
Maximizing the molecular information density requires simultaneously functionalizing distinct monomers and their coupling connections. However, current synthesis generally focuses on rather than reactions because multistep significantly escalate synthetic complexity in an exponential increase. Here, we report two-dimensional nanoarchitectures (2DNs) of end-on oligomers, with versatile structures negative differential resistance (NDR), synthesized by programmed surface-initiated step electrosynthesis based simultaneous utilization six including cross- homocouplings. The resulting vertically similar values thickness length, as crystalline 2DNs, exhibit subnanometer uniformity, ultrahigh compressive modulus 40 GPa, low-bias NDR at 0.13 V ultralow power consumption down to 0.05 nW/μm2. This highly controlled provides a unique dimension enhance structural diversity 2D nanomaterials for high-density low-power electronics.
Language: Английский
Citations
0
Chem, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 1, 2024
Language: Английский
Citations
0