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Journal articles on the topic 'Macromolecular Building Blocks'

Author: Grafiati

Published: 7 September 2023

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1

Cornelissen, Jeroen J. L. M., Alan E. Rowan, Roeland J. M. Nolte, and Nico A. J. M. Sommerdijk. "Chiral Architectures from Macromolecular Building Blocks." Chemical Reviews 101, no. 12 (December 2001): 4039–70. http://dx.doi.org/10.1021/cr990126i.

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2

Cornelissen, Jeroen J. L. M., Alan E. Rowan, Roeland J. M. Nolte, and Nico A. J. M. Sommerdijk. "ChemInform Abstract: Chiral Architectures from Macromolecular Building Blocks." ChemInform 33, no. 15 (May 22, 2010): no. http://dx.doi.org/10.1002/chin.200215294.

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3

Peruch, Frédéric, Jean-François Lahitte, F. Isel, and Pierre J. Lutz. "Macromonomers as well-defined building blocks in macromolecular engineering." Macromolecular Symposia 183, no. 1 (July 2002): 159–64. http://dx.doi.org/10.1002/1521-3900(200207)183:1<159::aid-masy159>3.0.co;2-7.

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4

Depoorter, Jérémy, Xibo Yan, Biao Zhang, Guillaume Sudre, Aurélia Charlot, Etienne Fleury, and Julien Bernard. "All poly(ionic liquid) block copolymer nanoparticles from antagonistic isomeric macromolecular blocks via aqueous RAFT polymerization-induced self-assembly." Polymer Chemistry 12, no. 1 (2021): 82–91. http://dx.doi.org/10.1039/d0py00698j.

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All-poly(ionic liquid) block copolymer nanoparticles are prepared by aqueous RAFT PISA using a couple of isomeric ionic liquid monomers leading to macromolecular building blocks with antagonistic solution behavior in water.

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5

Wouters, Staf M. L., David E. Clarke, Hiroki Noguchi, Steven De Feyter, and Arnout R. D. Voet. "SAKe: computationally designed modular protein building blocks for macromolecular assemblies." Acta Crystallographica Section A Foundations and Advances 77, a2 (August 14, 2021): C929. http://dx.doi.org/10.1107/s0108767321087705.

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6

TEZUKA, Yasuyuki. "Macromonomers and Telechelics: Building Blocks for Topologically Unique Macromolecular Structures." Kobunshi 45, no. 12 (1996): 862–67. http://dx.doi.org/10.1295/kobunshi.45.862.

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7

Inglis, Andrew J, Sebastian Sinnwell, Martina H Stenzel, and Christopher Barner-Kowollik. "Ultrafast Click Conjugation of Macromolecular Building Blocks at Ambient Temperature." Angewandte Chemie International Edition 48, no. 13 (February 18, 2009): 2411–14. http://dx.doi.org/10.1002/anie.200805993.

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8

Peng, Wentao, Yingying Cai, Luise Fanslau, and Philipp Vana. "Nanoengineering with RAFT polymers: from nanocomposite design to applications." Polymer Chemistry 12, no. 43 (2021): 6198–229. http://dx.doi.org/10.1039/d1py01172c.

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Reversible addition–fragmentation chain-transfer (RAFT) polymerization is a powerful tool for the precise formation of macromolecular building blocks that can be used for the construction of well-defined nanocomposites.

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9

Díez-Pascual, Ana M. "Hot Topics in 2022 and Future Perspectives of Macromolecular Science." Macromol 3, no. 1 (January 16, 2023): 28–33. http://dx.doi.org/10.3390/macromol3010002.

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10

Moldoveanu, Costel, Dorina Amariucai-Mantu, Violeta Mangalagiu, Vasilichia Antoci, Dan Maftei, Ionel I. Mangalagiu, and Gheorghita Zbancioc. "Microwave Assisted Reactions of Fluorescent Pyrrolodiazine Building Blocks." Molecules 24, no. 20 (October 18, 2019): 3760. http://dx.doi.org/10.3390/molecules24203760.

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We report here the synthesis and optical spectral properties of several new pyrrolodiazine derivatives. The luminescent heterocycles were synthesized by 1,3-dipolar cycloaddition reactions between N-alkylated pyridazine and methylpropiolate or dimethyl acetylenedicarboxylate (DMAD). The pyrrolopyridazine derivatives are blue emitters with moderate quantum yields (around 25%) in the case of pyrrolopyridazines and negligible yet measurable emission for pyrrolophthalazines. In a subsequent step towards including the pyrrolodiazine moiety, given its spectral properties in various macromolecular frameworks such as biological molecules, a subset of the synthetized compounds has been subjected to α-bromination. A selective and efficient way for α-bromination in heterogeneous catalysis of pyrrolodiazine derivatives under microwave (MW) irradiation is presented. We report substantially higher yields under MW irradiation, whereas the solvent amounts required are at least five-fold less compared to classical heating.

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11

Jutz, Günther, and Alexander Böker. "Bionanoparticles as functional macromolecular building blocks – A new class of nanomaterials." Polymer 52, no. 2 (January 2011): 211–32. http://dx.doi.org/10.1016/j.polymer.2010.11.047.

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12

Soler-Illia, Galo J. A. A., and Omar Azzaroni. "Multifunctional hybrids by combining ordered mesoporous materials and macromolecular building blocks." Chemical Society Reviews 40, no. 2 (2011): 1107. http://dx.doi.org/10.1039/c0cs00208a.

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13

van Nunen, J. L. M., A. P. H. J. Schenning, R. J. H. Hafkamp, C. F. van Nostrum, M. C. Feiters, and R. J. M. Nolte. "Design and synthesis of macromolecular structures from self-assembling building blocks." Macromolecular Symposia 98, no. 1 (July 1995): 483–90. http://dx.doi.org/10.1002/masy.19950980138.

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14

Otter, Ronja, and Pol Besenius. "Supramolecular assembly of functional peptide–polymer conjugates." Organic & Biomolecular Chemistry 17, no. 28 (2019): 6719–34. http://dx.doi.org/10.1039/c9ob01191a.

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The following review gives an overview about synthetic peptide–polymer conjugates as macromolecular building blocks and their self-assembly into a variety of supramolecular architectures, from supramolecular polymer chains, to anisotropic 1D arrays, 2D layers, and more complex 3D networks.

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15

Berki, Thomas R., Jonathan Martinelli, Lorenzo Tei, Helen Willcock, and Stephen J. Butler. "Polymerizable Gd(iii) building blocks for the synthesis of high relaxivity macromolecular MRI contrast agents." Chemical Science 12, no. 11 (2021): 3999–4013. http://dx.doi.org/10.1039/d0sc04750c.

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16

Kwan, Chak-Shing, Watson K. W. Ho, Yanyan Chen, Zongwei Cai, and Ken Cham-Fai Leung. "Synthesis of Functional Building Blocks for Type III-B Rotaxane Dendrimer." Polymers 13, no. 22 (November 12, 2021): 3909. http://dx.doi.org/10.3390/polym13223909.

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Second-generation type III-B rotaxane dendrons, equipped with succinimide and acetylene functional groups, were synthesized successfully and characterized by NMR spectroscopy and mass spectrometry. A cell viability study of a dendron with a normal cell line of L929 fibroblast cells revealed no obvious cytotoxicity at a range of 5 to 100 μM. The nontoxic properties of the sophisticated rotaxane dendron building blocks provided a choice of bio-compatible macromolecular machines that could be potentially developed into polymeric materials.

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17

Hughes, Matt D. G., Sophie Cussons, Najet Mahmoudi, David J. Brockwell, and Lorna Dougan. "Single molecule protein stabilisation translates to macromolecular mechanics of a protein network." Soft Matter 16, no. 27 (2020): 6389–99. http://dx.doi.org/10.1039/c9sm02484k.

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Folded globular proteins are attractive building blocks for biomaterials as their robust structures carry out diverse biological functions. These biomaterials are ideal to study the translation of molecular properties to multi-molecular assemblies.

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18

Daumann, Kevin, Patrick May, Janina Brückerhoff, and Mathias Ulbricht. "Synthesis of well-defined cross-linkable zwitterionic macromolecular building blocks for hydrogels." Reactive and Functional Polymers 131 (October 2018): 251–57. http://dx.doi.org/10.1016/j.reactfunctpolym.2018.07.004.

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19

Newkome, George R., Claus D. Weis, Charles N. Moorefield, Gregory R. Baker, Bradley J. Childs, and Jon Epperson. "Isocyanate-Based Dendritic Building Blocks: Combinatorial Tier Construction and Macromolecular-Property Modification." Angewandte Chemie International Edition 37, no. 3 (February 16, 1998): 307–10. http://dx.doi.org/10.1002/(sici)1521-3773(19980216)37:3<307::aid-anie307>3.0.co;2-l.

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20

Huang, Kui, Teresa A. Croce, Sharon K. Hamilton, Chinessa T. Adkins, Billie L. Evans, and Eva Harth. "Effective Drug Therapies from Functional, Macromolecular Building Blocks with a Biomimetic Design." Macromolecular Symposia 255, no. 1 (September 2007): 20–23. http://dx.doi.org/10.1002/masy.200750903.

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21

Privalov, Peter L. "Thermodynamic problems in structural molecular biology." Pure and Applied Chemistry 79, no. 8 (January 1, 2007): 1445–62. http://dx.doi.org/10.1351/pac200779081445.

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The most essential feature of living biological systems is their high degree of structural organization. The key role is played by two linear heteropolymers, the proteins and nucleic acids. Under environmental conditions close to physiological, these biopolymers are folded into unique native conformations, genetically determined by the arrangement of their standard building blocks. In their native conformation, biological macromolecules recognize their partners and associate with them, forming specific, higher-order complexes, the "molecular machines". Folding of biopolymers into their native conformation and their association with partners is in principle a reversible, thermodynamically driven process. Investigation of the thermodynamics of these basic biological processes has prime importance for understanding the mechanisms of forming these supra-macromolecular constructions and their functioning.

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22

Krywko-Cendrowska, Agata, Dawid Szweda, and Roza Szweda. "Well-Defined Conjugated Macromolecules Based on Oligo(Arylene Ethynylene)s in Sensing." Processes 8, no. 5 (May 3, 2020): 539. http://dx.doi.org/10.3390/pr8050539.

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Macromolecules with well-defined structures in terms of molar mass and monomer sequence became interesting building blocks for modern materials. The precision of the macromolecular structure makes fine-tuning of the properties of resulting materials possible. Conjugated macromolecules exhibit excellent optoelectronic properties that make them exceptional candidates for sensor construction. The importance of chain length and monomer sequence is particularly important in conjugated systems. The oligomer length, monomer sequence, and structural modification often influence the energy bang gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of the molecules that reflect in their properties. Moreover, the supramolecular aggregation that is often observed in oligo-conjugated systems is usually strongly affected by even minor structural changes that are used for sensor designs. This review discusses the examples of well-defined conjugated macromolecules based on oligo(arylene ethynylene) skeleton used for sensor applications. Here, exclusively examples of uniform macromolecules are summarized. The sensing mechanisms and importance of uniformity of structure are deliberated.

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23

Strasser, Paul, Marina Russo, Pauline Stadler, Patrick Breiteneder, Günther Redhammer, Markus Himmelsbach, Oliver Brüggemann, Uwe Monkowius, Petr Klán, and Ian Teasdale. "Green-light photocleavable meso-methyl BODIPY building blocks for macromolecular chemistry." Polymer Chemistry 12, no. 47 (2021): 6927–36. http://dx.doi.org/10.1039/d1py01245b.

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24

Boydston, Andrew J., and Christopher W. Bielawski. "Bis(imidazolylidene)s as modular building blocks for monomeric and macromolecular organometallic materials." Dalton Transactions, no. 34 (2006): 4073. http://dx.doi.org/10.1039/b607696n.

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25

Meijer, Michel D., Elwin de Wolf, Martin Lutz, Anthony L. Spek, Gerard P. M. van Klink, and Gerard van Koten. "C,N-2-[(Dimethylamino)methyl]phenylplatinum Complexes Functionalized with C60as Macromolecular Building Blocks." Organometallics 20, no. 20 (October 2001): 4198–206. http://dx.doi.org/10.1021/om010328g.

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26

Soler-Illia, Galo J. A. A., and Omar Azzaroni. "ChemInform Abstract: Multifunctional Hybrids by Combining Ordered Mesoporous Materials and Macromolecular Building Blocks." ChemInform 42, no. 25 (May 26, 2011): no. http://dx.doi.org/10.1002/chin.201125264.

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27

Percec, Virgil, Cheol-Hee Ahn, Wook-Dong Cho, Gary Johansson, and Douglas Schlueter. "Design of new macromolecular architectures by using quasi-equivalent monodendrons as building blocks." Macromolecular Symposia 118, no. 1 (June 1997): 33–43. http://dx.doi.org/10.1002/masy.19971180106.

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28

Harth, Eva, and Teresa A. Croce. "Carving Out Niches for Nanostructures: Implementation and Interplay of Building Blocks, Methods, and Tools." Australian Journal of Chemistry 59, no. 8 (2006): 525. http://dx.doi.org/10.1071/ch06245.

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The number and diversity of techniques to create well-defined polymeric architectures has set the foundation to reinvent macromolecular chemistry’s tenor. This development offers the chance to build refined structures with multifaceted, cross-disciplinary applications. We discuss a few advances in the design and development of selected nanoobjects with far-reaching potential. Herein, well-defined building blocks and introduced methods to establish three-dimensional architectures will be presented. Sequential attachment strategies and tools taken from biological chemistries achieve new levels of specificity.

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29

Wada, Yuya, Ken-ichi Shinohara, Hitoshi Asakawa, Sayaka Matsui, Tetsuya Taima, and Tomoyuki Ikai. "One-Step Synthesis of One-Dimensional Supramolecular Assemblies Composed of Helical Macromolecular Building Blocks." Journal of the American Chemical Society 141, no. 35 (August 13, 2019): 13995–4002. http://dx.doi.org/10.1021/jacs.9b07417.

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30

Ogoshi, Tomoki. "Hierarchical Materials from High Information Content Macromolecular Building Blocks: Construction, Dynamic Interventions, and Prediction." Chemical Reviews 123, no. 13 (July 12, 2023): 8041–43. http://dx.doi.org/10.1021/acs.chemrev.3c00355.

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31

Bačová, Petra, Dimitris G. Mintis, Eirini Gkolfi, and Vagelis Harmandaris. "Mikto-Arm Stars as Soft-Patchy Particles: From Building Blocks to Mesoscopic Structures." Polymers 13, no. 7 (April 1, 2021): 1114. http://dx.doi.org/10.3390/polym13071114.

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We present an atomistic molecular dynamics study of self-assembled mikto-arm stars, which resemble patchy-like particles. By increasing the number of stars in the system, we propose a systematic way of examining the mutual orientation of these fully penetrable patchy-like objects. The individual stars maintain their patchy-like morphology when creating a mesoscopic (macromolecular) self-assembled object of more than three stars. The self-assembly of mikto-arm stars does not lead to a deformation of the stars, and their shape remains spherical. We identified characteristic sub-units in the self-assembled structure, differing by the mutual orientation of the nearest neighbor stars. The current work aims to elucidate the possible arrangements of the realistic, fully penetrable patchy particles in polymer matrix and to serve as a model system for further studies of nanostructured materials or all-polymer nanocomposites using the mikto-arm stars as building blocks.

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32

Lutz, Jean-François. "Solution self-assembly of tailor-made macromolecular building blocks prepared by controlled radical polymerization techniques." Polymer International 55, no. 9 (2006): 979–93. http://dx.doi.org/10.1002/pi.2058.

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33

Tomalia, Donald A. "Birth of a new macromolecular architecture: dendrimers as quantized building blocks for nanoscale synthetic polymer chemistry." Progress in Polymer Science 30, no. 3-4 (March 2005): 294–324. http://dx.doi.org/10.1016/j.progpolymsci.2005.01.007.

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34

Katir, Nadia, Jean Pierre Majoral, Abdelkrim El Kadib, Anne-Marie Caminade, and Mostapha Bousmina. "Molecular and Macromolecular Engineering with Viologens as Building Blocks: Rational Design of Phosphorus-Viologen Dendritic Structures." European Journal of Organic Chemistry 2012, no. 2 (December 2, 2011): 269–73. http://dx.doi.org/10.1002/ejoc.201101376.

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35

Li, Min-Hui, and Patrick Keller. "Artificial muscles based on liquid crystal elastomers." Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 364, no. 1847 (August 21, 2006): 2763–77. http://dx.doi.org/10.1098/rsta.2006.1853.

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This paper presents our results on liquid crystal (LC) elastomers as artificial muscle, based on the ideas proposed by de Gennes. In the theoretical model, the material consists of a repeated series of main-chain nematic LC polymer blocks, N, and conventional rubber blocks, R, based on the lamellar phase of a triblock copolymer RNR. The motor for the contraction is the reversible macromolecular shape change of the chain, from stretched to spherical, that occurs at the nematic-to-isotropic phase transition in the main-chain nematic LC polymers. We first developed a new kind of muscle-like material based on a network of side-on nematic LC homopolymers. Side-on LC polymers were used instead of main-chain LC polymers for synthetic reasons. The first example of these materials was thermo-responsive, with a typical contraction of around 35–45% and a generated force of around 210 kPa. Subsequently, a photo-responsive material was developed, with a fast photochemically induced contraction of around 20%, triggered by UV light. We then succeeded in preparing a thermo-responsive artificial muscle, RNR, with lamellar structure, using a side-on nematic LC polymer as N block. Micrometre-sized artificial muscles were also prepared. This paper illustrates the bottom-up design of stimuli-responsive materials, in which the overall material response reflects the individual macromolecular response, using LC polymer as building block.

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36

Banerjee, Jayati, and Helena S. Azevedo. "Crafting of functional biomaterials by directed molecular self-assembly of triple helical peptide building blocks." Interface Focus 7, no. 6 (October 20, 2017): 20160138. http://dx.doi.org/10.1098/rsfs.2016.0138.

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Collagen is the most abundant extracellular matrix protein in the body and has widespread use in biomedical research, as well as in clinics. In addition to difficulties in the production of recombinant collagen due to its high non-natural imino acid content, animal-derived collagen imposes several major drawbacks—variability in composition, immunogenicity, pathogenicity and difficulty in sequence modification—that may limit its use in the practical scenario. However, in recent years, scientists have shifted their attention towards developing synthetic collagen-like materials from simple collagen model triple helical peptides to eliminate the potential drawbacks. For this purpose, it is highly desirable to develop programmable self-assembling strategies that will initiate the hierarchical self-assembly of short peptides into large-scale macromolecular assemblies with recommendable bioactivity. Herein, we tried to elaborate our understanding related to the strategies that have been adopted by few research groups to trigger self-assembly in the triple helical peptide system producing fascinating supramolecular structures. We have also touched upon the major epitopes within collagen that can be incorporated into collagen mimetic peptides for promoting bioactivity.

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37

Kim, Chan-Jin, Francesca Ercole, Yi Ju, Shuaijun Pan, Jingqu Chen, Yijiao Qu, John F. Quinn, and Frank Caruso. "Synthesis of Customizable Macromolecular Conjugates as Building Blocks for Engineering Metal–Phenolic Network Capsules with Tailorable Properties." Chemistry of Materials 33, no. 21 (October 29, 2021): 8477–88. http://dx.doi.org/10.1021/acs.chemmater.1c02912.

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38

Moorefield, Charles N., Anthony Schultz, and George R. Newkome. "From dendrimers to fractal polymers and beyond." Brazilian Journal of Pharmaceutical Sciences 49, spe (2013): 67–84. http://dx.doi.org/10.1590/s1984-82502013000700007.

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The advent of dendritic chemistry has facilitated materials research by allowing precise control of functional component placement in macromolecular architecture. The iterative synthetic protocols used for dendrimer construction were developed based on the desire to craft highly branched, high molecular weight, molecules with exact mass and tailored functionality. Arborols, inspired by trees and precursors of the utilitarian macromolecules known as dendrimers today, were the first examples to employ predesigned, 1 → 3 C-branched, building blocks; physical characteristics of the arborols, including their globular shapes, excellent solubilities, and demonstrated aggregation, combined to reveal the inherent supramolecular potential (e.g., the unimolecular micelle) of these unique species. The architecture that is a characteristic of dendritic materials also exhibits fractal qualities based on self-similar, repetitive, branched frameworks. Thus, the fractal design and supramolecular aspects of these constructs are suggestive of a larger field of fractal materials that incorporates repeating geometries and are derived by complementary building block recognition and assembly. Use of terpyridine-M2+-terpyridine (where, M = Ru, Zn, Fe, etc) connectivity in concert with mathematical algorithms, such as forms the basis for the Seirpinski gasket, has allowed the beginning exploration of fractal materials construction. The propensity of the fractal molecules to self-assemble into higher order architectures adds another dimension to this new arena of materials and composite construction.

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39

Denes, A. R., M. A. Tshabalala, R. Rowell, F. Denes, and R. A. Young. "Hexamethyldisiloxane-Plasma Coating of Wood Surfaces for Creating Water Repellent Characteristics." Holzforschung 53, no. 3 (May 10, 1999): 318–26. http://dx.doi.org/10.1515/hf.1999.052.

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Summary Southern yellow pine wood surfaces were modified under cold plasma conditions in order to create water repellent characteristics. The surface chemistry of the plasma “polymerized” hexamethyldisiloxane (PHMDSO) deposited onto wood surfaces was investigated using Electron Spectroscopy for Chemical Analysis (ESCA) and Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy (ATR-FTIR). The presence of a crosslinked macromolecular structure, based on Si-O-Si and Si-O-C linkages was detected. Pyrolysis Mass Spectroscopy (MS) was carried out to investigate the nature of the building blocks of the plasma generated macromolecular structure. Plasma modified samples exhibited very high water contact angle values (contact angle = 130 degrees) in comparison to the unmodified samples (contact angle ≤ 15 degrees), indicating the presence of a hydrophobic surface. Atomic Force Microscopy (AFM) images, collected both from unmodified and HMDSO-plasma modified samples, indicate the progressive growth of the plasma “polymer”, resulting in the deposition of a smooth layer at 10 minutes treatment time. Differential Thermal Analysis (DTA) indicated high thermal stability of the PHMDSO.

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40

Arshanitsa, Alexandr, Jevgenija Ponomarenko, Matiss Pals, Lilija Jashina, and Maris Lauberts. "Impact of Bark-Sourced Building Blocks as Substitutes for Fossil-Derived Polyols on the Structural, Thermal, and Mechanical Properties of Polyurethane Networks." Polymers 15, no. 17 (August 22, 2023): 3503. http://dx.doi.org/10.3390/polym15173503.

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The hydrophilic extractives isolated from black alder (Alnus glutinosa) bark through hot water extraction were characterized as novel renewable macromonomers capable of forming polyurethane (PU) networks based on a commercial polyisocyanate, with partial or complete replacement of petroleum-derived polyol polyether. The bark-sourced bio-polyol mainly consists of the xyloside form of the diarylheptanoid oregonin, along with oligomeric flavonoids and carbohydrates, resulting in a total OH group content of 15.1 mmol·g−1 and a molecular weight (Mn) of approximately 750 g∙mol−1. The 31P NMR data confirmed a similar proportion of aliphatic OH and phenolic groups. Three-component PU compositions were prepared using polyethylene glycol (Mn = 400 g∙mol−1), bio-polyol (up to 50%), and polymeric diphenylmethane diisocyanate, which were pre-polymerized in tetrahydrofuran (THF) solution with tin organic and tertiary amine catalysts. The resulting mixture was cast and subjected to thermal post-curing. Calculation and experimental data confirmed the crosslinking activity of the bark-sourced bio-polyol in PU, leading to an increase in glass transition temperature (Tg), a decrease in sol fraction yield upon leaching of cured PU networks in THF, a significant increase in Young’s modulus and tensile strength. The macromonomers derived from bark promoted char formation under high temperature and oxidative stress conditions, limiting heat release during macromolecular network degradation compared to bio-polyol-free PU. It was observed that amine catalysts, which are active in urethane formation with phenolic groups, promoted the formation of PU with higher Tg and modulus at tensile but with less limitation of heat liberation during PU macromolecular structure degradation. The high functionality of the bark-derived bio-polyol, along with the equal proportion of phenolic and aliphatic OH groups, allows for further optimization of PU characteristics using three variables: increasing the substitution extent of commercial polyethers, decreasing the NCO/OH ratio, and selecting the type of catalyst used.

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41

Percec, V., D. Schlueter, G. Ungar, S. Z. D. Cheng, and A. Zhang. "Hierarchical Control of Internal Superstructure, Diameter, and Stability of Supramolecular and Macromolecular Columns Generated from Tapered Monodendritic Building Blocks." Macromolecules 31, no. 6 (March 1998): 1745–62. http://dx.doi.org/10.1021/ma971459p.

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42

Morar, Cristina, Pedro Lameiras, Attila Bende, Gabriel Katona, Emese Gál, and Mircea Darabantu. "Design, synthesis and structure of novel G-2 melamine-based dendrimers incorporating 4-(n-octyloxy)aniline as a peripheral unit." Beilstein Journal of Organic Chemistry 14 (July 9, 2018): 1704–22. http://dx.doi.org/10.3762/bjoc.14.145.

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Background: 4-(n-Octyloxy)aniline is a known component in the elaboration of organic materials with mesogenic properties such as N-substituted Schiff bases, perylene bisimide assemblies with a number of 2-amino-4,6-bis[4-(n-octyloxy)phenylamino]-s-triazines, amphiphilic azobenzene-containing linear-dendritic block copolymers and G-0 monomeric or dimeric dendritic liquid crystals with photochromic azobenzene mesogens. The present ab initio study explores a previously unknown use of 4-(n-octyloxy)aniline in the synthesis, structure and supramolecular behaviour of new dendritic melamines. Results: Starting from 4-(n-octyloxy)aniline, seven G-2 melamine-based dendrimers were obtained in 29–79% overall yields. Their iterative convergent- and chemoselective synthesis consisted of SN2-Ar aminations of cyanuric chloride and final triple N-acylations and Williamson etherifications (→ G-2 covalent trimers) or stoichiometric carboxyl/amino 1:3 neutralisations (→ G-2 ionic trimers). These transformations connected G-1 chloro- and amino-termini dendrons to m-trivalent cores (triazin-2,4,6-triyl and benzene-1,3,5-triyl units) or tripodands (central building blocks), such as N-substituted melamines with 4-hydroxyphenyl or phenyl-4-oxyalkanoic motifs. Owing to the diversity of cores and central building blocks, the structural assortment of the dendritic series was disclosed by solvation effects (affecting reactivity), rotational stereodynamism and self-organisation phenomena (determining a vaulted and/or propeller macromolecular shape in solution). DFT calculations (in solution), (VT) NMR and IR (KBr) spectroscopy supported these assignments. TEM analysis revealed the ability of the title compounds towards self-assembling into homogeneously packed spherical nano-aggregates. Conclusions: The (non)covalent synthesis and step-by-step structural elucidation of novel G-2 melamine dendrimers based on 4-(n-octyloxy)aniline are reported. Our study demonstrates the crucial influence of the nature (covalent vs ionic) of the dendritic construction in tandem with that of its central building blocks on the aptitude of dendrimers to self-organise in solution and to self-assembly in the solid state.

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Veith, Michael, Hinka Hreleva-Caparrotti, Fadime Sahin, and Volker Huch. "[Al2(OH)8]2-Building Blocks Incorporated in Macromolecular Alumopolysiloxane Rings of the Type [O-SiPh2-O-SiPh2-O-Al+]n." Zeitschrift für anorganische und allgemeine Chemie 640, no. 5 (January 14, 2014): 863–67. http://dx.doi.org/10.1002/zaac.201300582.

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Katrusiak, Andrzej, Michalina Aniola, Kamil Dziubek, Kinga Ostrowska, and Ewa Patyk. "Biomolecular systems under pressure." Acta Crystallographica Section A Foundations and Advances 70, a1 (August 5, 2014): C1188. http://dx.doi.org/10.1107/s2053273314088111.

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Biological systems are often regarded as the ultimate goal of all knowledge in this respect that they can provide the clue for understanding the origin of life and the means for improving the life conditions and healthcare. Hence the interest in high-pressure behavior of organic and biomolecular systems. Such simple organic systems were among the first structural studies at high pressure at all. They included chloroform by Roger Fourme in 1968 [1] and benzene by Piermarini et al. in 1969, still with the use of photographic technique. The efficient studies on bio-macromolecular crystals had to wait for several decades till synchrotron radiation became more accessible and Roger Fourme again stood in the avant-garde of these studies [2]. At the turn of centuries his innovations in the laboratory equipment and experimental setup let him exploring high-pressure conformations of proteins, viral capsids and the double-helix molecular architecture in nucleic acids. These directions of high-pressure studies are continued for simple and macromolecular systems of biological importance. Recently new surprising facts were revealed about the compression of urea, sucrose, and other organic compounds, as well as of macromolecular crystals. Sugars are the main energy carriers for animals as well as building blocks in the living tissue, they are also ideal models for studying pressure-induced changes of OH···O and CH···O interactions. Different types of transformations occur in compressed urea, the first organic compound synthesized in laboratory. Hen egg-white lysozyme was investigated at moderate pressure in a beryllium vessel and the compression of both tetragonal and orthorhombic modifications were measured to 1.0 GPa in a DAC; the high-pressure structure of the tetragonal form was determined and refined at still higher pressure by Fourme et al. [3] Can high pressure provide information about the remarkable polymorphism of lysozyme?

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Vlăsceanu, George Mihail, Mariana Ioniță, Corina Cristiana Popescu, Elena Diana Giol, Irina Ionescu, Andrei-Mihai Dumitrașcu, Mădălina Floarea, et al. "Chitosan-Based Materials Featuring Multiscale Anisotropy for Wider Tissue Engineering Applications." International Journal of Molecular Sciences 23, no. 10 (May 10, 2022): 5336. http://dx.doi.org/10.3390/ijms23105336.

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We designed graphene oxide composites with increased morphological and structural variability using fatty acid-coupled polysaccharide co-polymer as the continuous phase. The matrix was synthesized by N, O-acylation of chitosan with palmitic and lauric acid. The obtained co-polymer was crosslinked with genipin and composited with graphene oxide. FTIR spectra highlighted the modification and multi-components interaction. DLS, SEM, and contact angle tests demonstrated that the conjugation of hydrophobic molecules to chitosan increased surface roughness and hydrophilicity, since it triggered a core-shell macromolecular structuration. Nanoindentation revealed a notable durotaxis gradient due to chitosan/fatty acid self-organization and graphene sheet embedment. The composited building blocks with graphene oxide were more stable during in vitro enzymatic degradation tests and swelled less. In vitro viability, cytotoxicity, and inflammatory response tests yielded promising results, and the protein adsorption test demonstrated potential antifouling efficacy. The robust and stable substrates with heterogeneous architecture we developed show promise in biomedical applications.

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Nguyen, Michel, Khalid Ferji, Sébastien Lecommandoux, and Colin Bonduelle. "Amphiphilic Nucleobase-Containing Polypeptide Copolymers—Synthesis and Self-Assembly." Polymers 12, no. 6 (June 16, 2020): 1357. http://dx.doi.org/10.3390/polym12061357.

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Nucleobase-containing polymers are an emerging class of building blocks for the self-assembly of nanoobjects with promising applications in nanomedicine and biology. Here we present a macromolecular engineering approach to design nucleobase-containing polypeptide polymers incorporating thymine that further self-assemble in nanomaterials. Diblock and triblock copolypeptide polymers were prepared using sequential ring-opening polymerization of γ-Benzyl-l-glutamate N-carboxyanhydride (BLG-NCA) and γ-Propargyl-l-glutamate N-carboxyanhydride (PLG-NCA), followed by an efficient copper(I)-catalyzed azide alkyne cycloaddition (CuAAc) functionalization with thymidine monophosphate. Resulting amphiphilic copolymers were able to spontaneously form nanoobjects in aqueous solutions avoiding a pre-solubilization step with an organic solvent. Upon self-assembly, light scattering measurements and transmission electron microscopy (TEM) revealed the impact of the architecture (diblock versus triblock) on the morphology of the resulted nanoassemblies. Interestingly, the nucleobase-containing nanoobjects displayed free thymine units in the shell that were found available for further DNA-binding.

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Doblin, Monika S., Filomena Pettolino, and Antony Bacic. "Plant cell walls: the skeleton of the plant world." Functional Plant Biology 37, no. 5 (2010): 357. http://dx.doi.org/10.1071/fp09279.

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Plants are our major source of renewable biomass. Since cell walls represent some 50% of this biomass, they are major targets for biotechnology. Major drivers are their potential as a renewable source of energy as transport fuels (biofuels), functional foods to improve human health and as a source of raw materials to generate building blocks for industrial processes (biobased industries). To achieve sustainable development, we must optimise plant production and utilisation and this will require a complete understanding of wall structure and function at the molecular/biochemical level. This overview summarises the current state of knowledge in relation to the synthesis and assembly of the wall polysaccharides (i.e. the genes and gene families encoding the polysaccharide synthases and glycosyltransferases (GlyTs)), the predominant macromolecular components. We also touch on an exciting emerging role of the cell wall–plasma membrane–cytoskeleton continuum as a signal perception and transduction pathway allowing plant growth regulation in response to endogenous and exogenous cues.

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Yamamoto, Kimihisa. "(Invited, Digital Presentation) Synthesis of Multi-Metallic Clusters Using a Dendrimer Reactor." ECS Meeting Abstracts MA2022-01, no. 13 (July 7, 2022): 931. http://dx.doi.org/10.1149/ma2022-0113931mtgabs.

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Dendrimers are highly branched organic macromolecules with successive layers or “generations” of branch units surrounding a central core. Organic inorganic hybrid versions have also been produced, by trapping metal ions or metal clusters within the voids of the dendrimers. Their unusual, tree-like topology endows these nanometer-sized macromolecules with a gradient in branch density from the interior to the exterior, which can be exploited to direct the transfer of charge and energy from the dendrimer periphery to its core. We show that tinchloride, SnCl2 and FeCl3 complexes to the imines groups of a spherical polyphenylazomethine dendrimer in a stepwise fashion according to an electron gradient, with complexation in a more peripheral generation proceeding only after complexation in generations closer to the core has been completed. By attaching an electron-withdrawing group to the dendrimer core, we are able to change the complexation pattern, so that the core imines are complexed last. By further extending this strategy, it should be possible to control the number and location of metal ions incorporated into dendrimer structures, which might and uses as tailored catalysts, building blocks, or fine-controlled clusters for advanced materials. The metal-assembly in a discrete molecule can be converted to a size-regulated metal particle with a size smaller than 1 nm as a molecular reactor. Due to the well-defined number of metal clusters in the subnanometer size region, its property is much different from that of bulk or general metal nanoparticles. The chemistry of metal clusters on the sub-nanometer scale is not yet well understood because metal clusters, especially multi-metallic clusters, are difficult to synthesize with control over size and composition. The template synthesis of multi-metallic sub-nanoclusters is achieved using a phenylazomethine dendrimer as a macromolecular template.

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Raval, R. "Molecular assembly at surfaces: progress and challenges." Faraday Discuss. 204 (2017): 9–33. http://dx.doi.org/10.1039/c7fd90072d.

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Molecules provide versatile building blocks, with a vast palette of functionalities and an ability to assemble via supramolecular and covalent bonding to generate remarkably diverse macromolecular systems. This is abundantly displayed by natural systems that have evolved on Earth, which exploit both supramolecular and covalent protocols to create the machinery of life. Importantly, these molecular assemblies deliver functions that are reproducible, adaptable, finessed and responsive. There is now a real need to translate complex molecular systems to surfaces and interfaces in order to engineer 21st century nanotechnology. ‘Top-down’ and ‘bottom-up’ approaches, and utilisation of supramolecular and covalent assembly, are currently being used to create a range of molecular architectures and functionalities at surfaces. In parallel, advanced tools developed for interrogating surfaces and interfaces have been deployed to capture the complexities of molecular behaviour at interfaces from the nanoscale to the macroscale, while advances in theoretical modelling are delivering insights into the balance of interactions that determine system behaviour. A few examples are provided here that outline molecular behaviour at surfaces, and the level of complexity that is inherent in such systems.

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Calvino, Celine. "Photocycloadditions for the Design of Reversible Photopolymerizations." CHIMIA 76, no. 10 (October 26, 2022): 816. http://dx.doi.org/10.2533/chimia.2022.816.

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The quest for circular designs and ways to reuse polymer materials demands further advances in the development of reversible chemistries. Stimuli-responsive systems incorporated into polymer materials that enable the formation and cleavage of covalent bonds, hold great potential to reversibly decompose materials into their original building blocks. [2π+2π] photocycloadditions, for which the addition and reversion mechanism can be triggered by disparate wavelengths, stand as an attractive platform for triggering such controlled and reversible photoligation towards achieving renewable polymer materials. This perspective highlights the potential of this type of photochemistry to incorporate solid polymer materials and generate reversible polymerizations. The design of effective photoresponsive materials with specific functions requires the consideration of a number of parameters. Following a bottom-up approach – from molecular chemistry to macromolecular functionality – this perspective provides a recipe of the key aspects to consider in the design of such advanced renewable materials. Furthermore, examples of the state of the art in the field are highlighted and an overview of the fundamental challenges that remain is provided. Finally, an outlook on the next frontiers to cross is proposed.

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