Article
Chemistry, Organic
Manuel A. Martinez, Daniel Aranda, Enrique Orti, Juan Arago, Luis Sanchez
Summary: The self-assembling features of amphiphilic N-annulated perylene bisimides (N-PBIs) 1-4 in water were investigated experimentally and theoretically. The hydrophilic/hydrophobic ratio, determined by the oligo(ethylene) glycol (OEG) chains in the monomers, plays a significant role in the enthalpy of self-assembly. Molecular dynamic simulations revealed the influence of the initial arrangement of hydrophilic side chains and water-side chain interactions on the enthalpy contribution and overall stability of the aggregated species in water.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Tian Tian, Duo Wei, Lingling Ge, Zhifeng Wang, Chong Chen, Rong Guo
Summary: Based on the hypothesis of utilizing photoinduced electron transfer, one-dimensional organic nanomaterials with tunable donor-acceptor interfaces provide a promising avenue to achieve high optoelectric properties. Experimental results show that delicately tuned hydrogen bonds and pi-pi interactions can lead to the formation of assemblies with diverse microstructures, and the photoelectric performances are strongly dependent on the molecular arrangement within the nanomaterials.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Chemistry, Inorganic & Nuclear
Hailong Yan, Jinbing Cheng, Zuxue Bai, Tao Peng, Yang Lu, Jang-Kyo Kim, Yongsong Luo
Summary: In this study, a NiMn2O4@MXene composite with a crumpled surface was fabricated by a hydrothermal method and developed dip-coating method, resulting in improved electrode specific capacitance and retention rate. Additionally, an asymmetrical device was assembled, demonstrating ultra-high energy density.
DALTON TRANSACTIONS
(2021)
Article
Engineering, Environmental
Zheng Fang, Yang Liu, Ping Chen, Daguang Li, Haijin Liu, Zhenjun Xiao, Yixun Zheng, Zifeng Lin, Jin Luo, Wenying Lv, Guoguang Liu
Summary: In this study, carbon quantum dots-doped perylene diimide supramolecular nanofibers were synthesized and demonstrated to have efficient catalytic activity in the photocatalytic degradation of naproxen. The degradation mechanism and influencing factors were investigated, providing fundamental data for the remediation of contaminants in water and wastewater. Additionally, a PDI/CQDs cellulose acetate membrane was synthesized and its stability and efficiency were evaluated under different water conditions.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Multidisciplinary Sciences
Yuzhu Ma, Hongjin Zhang, Runfeng Lin, Yan Ai, Kun Lan, Linlin Duan, Wenyao Chen, Xuezhi Duan, Bing Ma, Changyao Wang, Xiaomin Li, Dongyuan Zhao
Summary: In this study, a nanodroplet remodeling strategy is proposed for the synthesis of hierarchical multi-chambered mesoporous silica nanoparticles with tunable architectures. The dual-chambered nanoparticles have a high surface area and two interconnected cavities, allowing for separate anchoring of multiple species without mutual interference. Additionally, the dual-chambered mesoporous nanoreactors prepared using this strategy exhibit efficient mass transfer, leading to improved selectivity of the target product.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yuting Bi, Caikun Cheng, Zongze Zhang, Rongjuan Liu, Jingjing Wei, Zhijie Yang
Summary: In this work, the authors demonstrate the coupling of molecular self-assembly kinetics with the colloidal self-assembly kinetics of inorganic nanoparticles, leading to the formation of hierarchically assembled tubular nanocomposites with distinct structures. By serving as artificial histones, the colloidal nanoparticles promote the formation of single layered nanotubes and resistant tubular nanocomposites. Alternatively, aggregated nanoparticles are encapsulated into double-layer supramolecular nanotubes, resulting in nanoparticle superlattices with open channels. Increasing the amounts of nanoparticles enables the assembly into pseudohexagonal superlattices and triple-layered tubular nanocomposites. The sense of helicity transfers from the supramolecular nanotubes to the nanoparticle superlattices. These findings provide a strategy for designing and controlling hierarchical assembly between supramolecular chemistry and inorganic solids.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Mauro Cainelli, Raffaele Borrelli, Yoshitaka Tanimura
Summary: In this theoretical study, we investigated the effect of mixed Frenkel and charge transfer states on the spectral properties of perylene bisimide derivatives, focusing on the role of strong electron-phonon interactions. The results show that the inclusion of charge transfer states promotes the localization of excitons, leading to a decrease in the intensity of the hot state peak and the 0-1 peak and an increase in the intensity of the 0-0 emission peak, resulting in a decrease in the coherence length of excitons.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Wenlong Huo, Elena Tervoort, Silvan Gantenbein, Etienne Jeoffroy, Jinlong Yang, Andre R. Studart
Summary: This study reports a cost-effective and simple process to create strong, highly porous ceramics via direct ink writing of suspensions of hollow microspheres into cellular architectures with pores at three hierarchical levels. X-ray diffraction, rheological measurements, scanning electron microscopy, and mechanical tests are conducted to thoroughly study the processing steps and morphology of the printed hierarchical porous ceramics. The presence of pores at multiple length scales significantly increases the mechanical strength of the porous structure, providing a useful platform for the manufacturing of lightweight ceramics from inexpensive and widely available feedstock materials.
ADVANCED MATERIALS TECHNOLOGIES
(2023)
Article
Energy & Fuels
Dingfu Zhang, Jiaxin Yao, Guiling Wang, Jinling Yin, Kai Zhu, Jun Yan, Dianxue Cao, Min Zhu
Summary: Hydrogen (H-2) plays a key role in promoting a sustainable low-carbon economy and addressing energy security. This study successfully prepared p-Ni x Co9-x S8 catalyst with polyvinylpyrrolidone (PVP) compounds, which exhibited a hierarchical flowerlike nanosheet structure. The p-Ni x Co9-x S8 nanosheets showed outstanding HER performance due to their ultrathin and porous surface, enabling rapid electrolyte injection and providing abundant active sites for H(+) adsorption.
Article
Chemistry, Inorganic & Nuclear
Leiyun Han, Xilong Liu, Zheng Cui, Yingjie Hua, Chongtai Wang, Xudong Zhao, Xiaoyang Liu
Summary: In this study, hierarchical copper cobalt sulfide nanobelt array structures with well-defined morphology control were successfully synthesized as high energy density electrode materials for asymmetric supercapacitors. By controlling the reaction time and sulfide ion concentration during the sulfidation reactions, saturated sulfidation was achieved while maintaining the morphology, structural integrity, and stability of the precursor. The CuCo2S4 electrode exhibited a high specific capacity, excellent cycling stability, and high energy density in an aqueous asymmetric device, showing potential for use in high-performance energy storage devices.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Review
Chemistry, Multidisciplinary
Yutao Sang, Minghua Liu
Summary: This article discusses the importance of using asymmetry to manipulate molecular-level devices and hierarchical functional materials, focusing on how chirality can be utilized to design and evolve highly ordered and complex nanostructures through self-assembly, as well as the future prospects of chiral nanostructures.
Article
Engineering, Electrical & Electronic
Yu Zhao, Shang Xiang, Jiaqi Han, Long Li
Summary: The hierarchical pattern exploitation (HPE) method is proposed for efficient electromagnetic analysis of finite periodic arrays. HPE accelerates the matrix assembly and reduces storage space by partitioning the array hierarchically and taking advantage of repeating patterns. Numerical examples demonstrate that HPE outperforms classical methods in terms of storage and CPU time, and it also shows competitive performance compared to other commonly used algorithms.
IEEE TRANSACTIONS ON ANTENNAS AND PROPAGATION
(2022)
Article
Chemistry, Physical
Zhiqiang Zhao, Zheng Bian, Yu Chen, Chuanqing Kang, Lianxun Gao, Guangshan Zhu
Summary: The study shows that chiral oligomers can self-assemble into vesicle-like particles in hydrophobic or hydrophilic solvent systems independently of molecular design and chemical environments. The vesicular membranes are likely stabilized by pi-pi stacking interactions between foldamer backbones and collective van der Waals interactions between side chains, as supported by TEM, UV, CD and PXRD data.
Article
Chemistry, Multidisciplinary
Yuefei Wang, Qing Li, Jiaxing Zhang, Wei Qi, Shengping You, Rongxin Su, Zhimin He
Summary: This study reports the self-templated assembly of amyloid-like dipeptides into long-range-ordered hierarchical helical arrays through spontaneous fibrillization and hierarchical helical assembly within a confined film. By changing the chirality and enantioselective interactions, researchers can precisely control the phase behavior, handedness, and chiroptics of the self-assembled HHAs. The redox activity of HHAs allows for the in situ decoration of nanoparticles with high catalytic activity.
Article
Biochemistry & Molecular Biology
Srijeeb Karmakar, Arjun Sankhla, Vimal Katiyar
Summary: The holo form of Cytochrome-C remains structurally intact in the presence of heme, but prolonged thermal and pH stress can lead to dissociation of heme, resulting in the collapse of the protein structure into a macromolecular amyloid-network and FeQDs with 2-3 nm diameter. Further studies revealed that FeQDs can re-adsorb on the surface of the amyloid network, forming a FeQD-decorated amyloid matrix. Excitingly, the FeQDs exhibit gel-like properties and support cell growth without cytotoxicity, suggesting potential for diverse biological applications as advanced biomaterials.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2021)
Article
Polymer Science
Yanlin Shi, Sung-Po R. Chen, George Fragkiadakis, Daniele Parisi, Virgil Percec, Dimitris Vlassopoulos, Michael J. Monteiro
Summary: The shape, breadth, and average molecular weight of the overall molecular weight distribution (MWD) are important for determining polymer properties. Traditional methods can only achieve desired Gaussian distribution through complex modeling, while living radical polymerization provides a simpler route. Blending low-reactive RAFT agents allows the construction of square, slanted, and chair-like MWDs, providing control over MWD shape and breadth. This blending method overcomes difficulties in producing unusual MWDs and offers a general synthetic strategy for studying structure-property relationships of polymers.
Article
Polymer Science
Virgil Percec, Dipankar Sahoo, Jasper Adamson
Summary: This article organized for the first time the stimuli-responsive principles of supramolecular organizations emerging from self-assembling and self-organizable dendrons, dendrimers, and dendronized polymers, which is fundamental to natural and life sciences.
Article
Polymer Science
Adrian Moreno, Gerard Lligadas, Jasper Adamson, Devendra S. Maurya, Virgil Percec
Summary: The Nobel Prize in Chemistry for 2022 was awarded to Bertozzi, Meldal, and Sharpless for their contribution to the development of click chemistry and biorthogonal chemistry. Since 2001, when click chemistry was proposed by Sharpless's laboratory, synthetic chemists have favored click reactions as a preferred method to create new functions. This perspective summarizes the research conducted in our laboratories on CuAAC, TBC, and TERMINI click reactions, and their applications in assembling complex macromolecules and self-organizations with biological relevance.
Article
Pharmacology & Pharmacy
Juncheng Lu, Elena N. Atochina-Vasserman, Devendra S. Maurya, Muhammad Irhash Shalihin, Dapeng Zhang, Srijay S. Chenna, Jasper Adamson, Matthew Liu, Habib Ur Rehman Shah, Honey Shah, Qi Xiao, Bryn Queeley, Nathan A. Ona, Erin K. Reagan, Houping Ni, Dipankar Sahoo, Mihai Peterca, Drew Weissman, Virgil Percec
Summary: The use of viral and synthetic vectors for nucleic acid delivery is crucial for the rapid development of effective COVID-19 vaccines. Lipid nanoparticles (LNPs) composed of phospholipids, PEG-conjugated lipids, cholesterol, and ionizable lipids have been employed as the leading nonviral delivery vector for COVID-19 mRNA vaccines by BioNTech/Pfizer and Moderna. In this study, a methodology involving screening libraries was used to discover the molecular design principles necessary for targeted mRNA delivery to specific organs, using a one-component ionizable multifunctional amphiphilic Janus dendrimer (IAJD) derived from plant phenolic acids. These design principles simplify the synthesis of IAJDs and the assembly of monodisperse dendrimersome nanoparticles (DNPs) with predictable dimensions, ultimately enhancing accessibility to diverse mRNA-based vaccines and nanotherapeutics.
Article
Chemistry, Multidisciplinary
Dipankar Sahoo, Emad Aqad, Mihai Peterca, Virgil Percec
Summary: This publication reports the structural analysis of the 3D self-organizations of HATn molecules, revealing the formation of highly ordered helical and nonhelical pyramidal and discotic columns. It demonstrates that a single building block can self-organize into different assemblies via its constitutional isomers. The findings raise important questions about the current understanding of helical self-organizations.
Article
Chemistry, Multidisciplinary
Dipankar Sahoo, Emad Aqad, Mihai Peterca, Virgil Percec
Summary: The molecular structures of 3D crystal and 2D liquid crystal phases of discotic molecules have never been determined at the molecular level. This study investigates the molecular structure of HATn self-organizations and presents the molecular structures of HAT4 in its crystal and liquid crystal states.
Article
Chemistry, Multidisciplinary
Juncheng Lu, Elena N. Atochina-Vasserman, Devendra S. Maurya, Dipankar Sahoo, Nathan Ona, Erin K. Reagan, Houping Ni, Drew Weissman, Virgil Percec
Summary: Researchers have developed a one-component multifunctional sequence-defined ionizable amphiphilic Janus dendrimer (IAJD) delivery system for mRNA. The IAJDs coassemble with mRNA into predictable-size vesicles called dendrimersome nanoparticles (DNPs) by simple injection. Rapid coassembly with mRNA and in vivo screening led to the discovery of the most active IAJDs targeting specific organs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Virgil Percec, Dipankar Sahoo, Devendra S. Maurya
Summary: This paper discusses the challenges and latest developments in fluorine chemistry, highlighting the bridging role of fluorine and fluorous chemistry in various scientific fields. The reactivity of fluoride as a leaving group and the use of fluorinated reagents in different reactions are illustrated. The synthesis of poly(etherketone)s and the self-assembly of supramolecular structures are among the topics explored. The importance of fluorinated amino acids, peptides, and semifluorinated amphiphilic Janus dendrimers in biological systems is also discussed.