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1. Production and Characterization of Cellulose Nanofiber Slurries and Sheets for Biomedical Applications

   https://doi.org/10.3389/fnano.2021.729743  

   Carter, Nicklaus; Grant, Isabelle; Dewey, Marley; Bourque, Mary; Neivandt, David J. (December 2021, Frontiers in Nanotechnology)

   Cellulose nanomaterials are produced employing a multitude of methodologies including electrospinning, bacterial generation, acid digestion, and a variety of mechanical defibrillation techniques; the morphology of the nanomaterial produced is specific to the production process. Feedstocks range from various forms of woody biomass, to fungi, and have a great impact on the resulting product. The mechanical defibrillation technique, such as that employed in the present work, continuously breaks down cellulose fibers suspended in water via segmentation and defibrillation through grinding and refining. The process is typically operated until a desired level of fines is achieved in the resultant slurry of cellulose nanofiber (CNF), alternatively known as cellulose nanofibril. Mechanical defibrillation processes can be built to produce several liters in a small batch system or up to tons per day in a continuous pilot scale refiner system. In the present work a continuous system was developed with the capacity to produce 14 L of cellulose nanofiber slurry with consistent specifications and in a manner compliant with GMP/GLP protocols in order to be amenable to biomedical applications. The system was constructed within an ISO class 7 cleanroom and refining was performed on bleached softwood pulp suspension in purified water. This manuscript details the continuous grinding system, the processes employed to produce cellulose nanofiber, and characterizes the resultant cellulose nanofiber slurry and sheets formed from the slurry. 

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2. Structure and Morphology of Poly(lactic acid) Stereocomplex Nanofiber Shish Kebabs

   https://doi.org/10.1021/acsmacrolett.9b00953  

   Xie, Qing; Chang, Xiaohua; Qian, Qian; Pan, Pengju; Li, Christopher Y. (January 2020, ACS Macro Letters)
3. Multiferroicity and Semi‐Cylindrical Alignment in Janus Nanofiber Aggregates

   https://doi.org/10.1002/adfm.202412690  

   Arash, Saba; Kharal, Govinda; Chavez, Bryan_L; Ferson, Noah_D; Mills, Sara_C; Andrew, Jennifer_S; Crawford, Thomas_M; Wu, Yanwen (November 2024, Advanced Functional Materials)

   Abstract 1D multiferroic fibers are known to exhibit attractive characteristics, including enhanced magnetoelectric (ME) coupling compared to thin film and bulk architectures. A comprehensive understanding of composite fibers, however, has been hindered by the complexity of their structure, leading to limited reports. Here, clear and strong ME coupling is experimentally detected in a composite Janus nanofiber aggregate using second harmonic generation (SHG) polarimetry under different magnetic field orientations. The observation of such a pronounced effect using an all‐optical method has not been previously reported in multiferroic fibers. A series of global fits is performed to the SHG polarimetry results to investigate the behavior of nanofibers within an aggregate. We find the magnetically assembled fibers exhibit semi‐cylindrical alignment as well as the expected lengthwise alignment despite variations in size and composition from fiber to fiber. The ME coupling and the semi‐cylindrical alignment seen in SHG are further corroborated via X‐ray diffraction under similar magnetic field conditions. These findings contribute to the development of complex composite and multifunctional devices using multiferroic nanostructures as building blocks, even those with inhomogeneous shapes and geometries. 

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4. Anatomy of a selectively coassembled β-sheet peptide nanofiber

   https://doi.org/10.1073/pnas.1912810117  

   Shao, Qing; Wong, Kong M.; Seroski, Dillon T.; Wang, Yiming; Liu, Renjie; Paravastu, Anant K.; Hudalla, Gregory A.; Hall, Carol K. (February 2020, Proceedings of the National Academy of Sciences)

   Peptide self-assembly, wherein molecule A associates with other A molecules to form fibrillar β-sheet structures, is common in nature and widely used to fabricate synthetic biomaterials. Selective coassembly of peptide pairs A and B with complementary partial charges is gaining interest due to its potential for expanding the form and function of biomaterials that can be realized. It has been hypothesized that charge-complementary peptides organize into alternating ABAB-type arrangements within assembled β-sheets, but no direct molecular-level evidence exists to support this interpretation. We report a computational and experimental approach to characterize molecular-level organization of the established peptide pair, CATCH. Discontinuous molecular dynamics simulations predict that CATCH(+) and CATCH(−) peptides coassemble but do not self-assemble. Two-layer β-sheet amyloid structures predominate, but off-pathway β-barrel oligomers are also predicted. At low concentration, transmission electron microscopy and dynamic light scattering identified nonfibrillar ∼20-nm oligomers, while at high concentrations elongated fibers predominated. Thioflavin T fluorimetry estimates rapid and near-stoichiometric coassembly of CATCH(+) and CATCH(−) at concentrations ≥100 μM. Natural abundance¹³C NMR and isotope-edited Fourier transform infrared spectroscopy indicate that CATCH(+) and CATCH(−) coassemble into two-component nanofibers instead of self-sorting. However,¹³C–¹³C dipolar recoupling solid-state NMR measurements also identify nonnegligible AA and BB interactions among a majority of AB pairs. Collectively, these results demonstrate that strictly alternating arrangements of β-strands predominate in coassembled CATCH structures, but deviations from perfect alternation occur. Off-pathway β-barrel oligomers are also suggested to occur in coassembled β-strand peptide systems. 

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5. Co-assembly of a multicomponent network of nanofiber-wrapped nanotubes

   https://doi.org/10.1039/D1NR08508E  

   Mason, McKensie L.; Lin, Tao; Linville, Jenae J.; Parquette, Jon R. (March 2022, Nanoscale)

   Strategies to create organized multicomponent nanostructures composed of discrete, self-sorted domains are important for developing materials that mimic the complexity and multifunctionality found in biological systems. These structures can be challenging to achieve due to the required balance of molecular self-recognition and supramolecular attraction needed between the components. Herein, we report a strategy to construct a two-component nanostructure via a hierarchical assembly process whereby two monomeric building blocks undergo self-sorting assembly at the molecular level followed by a supramolecular association to form a nanofiber-wrapped nanotube. The two molecules self-sorted into respective nanofiber and nanotube assemblies, yet assembly of the nanofibers in the presence of the nanotube template allowed for directed integration into a hierarchical multilayer structure via electrostatic interactions. The fiber-wrapped nanotube co-assembly was characterized using transmission electron microscopy (TEM), atomic force microscopy (AFM) and Förster resonance energy transfer (FRET) between the components. Strategies to co-assemble multicomponent nanostructures composed of discrete, spatially sorted domains with controllable higher level interactions will be critical for the development of novel, functionally competent nanomaterials. 

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