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Despite being a pillar of high‐performance materials in industry, manufacturing carbon fiber composites with simultaneously enhanced multifunctionality and structural properties has remained elusive due to the lack of practical bottom‐up approaches with control over nanoscale interactions. Guided by the droplet's internal currents and amphiphilicity of nanomaterials, herein, a programmable spray coating is introduced for the deposition of multiple nanomaterials with tailorable patterns in composite.  It is shown that such patterns regulate the formation of interfaces, damage containment, and electrical‐thermal conductivity of the composites, which is absent in conventional manufacturing that primarily rely on incorporating nanomaterials to achieve specific functionalities. Molecular dynamics simulations show that increasing the hydrophilicity of the hybrid nanomaterials, which is synchronous with shifting patterns from disk to ring, improves the interactions between the carbon surfaces and epoxy at the interfaces,manifested in enhanced interlaminar and flexural performance. Transitioning from ring to disk creates a larger interconnected network  leading to improved thermal and electrical properties without penalty in mechanical properties. This novel approach introduces a new design , where the mechanical and multifunctional performance is controlled by the shape of the deposited patterns, thus eliminating the trade‐off between properties that are considered paradoxical in today's manufacturing of hierarchical composites.

 

Dispersing carbon nanomaterials in solvents is effective in transferring their significant mechanical and functional properties to polymers and nanocomposites. However, poor dispersion of carbon nanomaterials impedes exploiting their full potential in nanocomposites. Cellulose nanocrystals (CNCs) are promising for dispersing and stabilizing pristine carbon nanotubes (pCNTs) and graphene nanoplatelets (pGnP) in protic media without functionalization. Here, the underlying mechanisms at the molecular level are investigated between CNC and pCNT/pGnP that stabilize their dispersion in polar solvents. Based on the spectroscopy and microscopy characterization of CNCpCNT/pGnP and density functional theory (DFT) calculations, an additional intermolecular mechanism is proposed between CNC and pCNT/pGnP that forms carbonoxygen covalent bonds between hydroxyl end groups of CNCs and the defected sites of pCNTs/pGnPs preventing re‐agglomeration in polar solvents. This work's findings indicate that the CNC‐assisted process enables new capabilities in harnessing nanostructures at the molecular level and tailoring the performance of nanocomposites at higher length scales.

 

Carbon fiber-based structural lithium-ion batteries are attracting significant attention in the automotive and aerospace industries due to their dual capability of energy storage and mechanical load-bearing, leading to weight reduction. These batteries utilize lightweight carbon fiber (CF) composites, which offer excellent stiffness, strength-to-weight ratios, and electrical conductivity. Polyacrylonitrile-based CFs, comprising graphitic and amorphous carbon, are particularly suitable for Li-ion battery applications as they allow the storage of lithium ions. However, integrating lithium iron phosphate (LFP) into CFs poses challenges due to complex lab-scale processes and the use of toxic dispersants, hindering large-scale industrial compatibility. To address this, we investigate the development of water-based LFP-integrated CF structural Li-ion batteries. Homogeneous suspensions are created using cellulose nanocrystals (CNCs) to form hybrid structures. The battery system employs LFP-modified CF as the cathode, unsized CF as the anode, and a water-based electrolyte. The LFP-CNC-graphene nanoplatelet (GNP) hybrids are coated onto CFs through immersion coating. Scanning electron microscopy (SEM) images confirm the well-dispersed and well-adhered LFP-CNC-GNP structures on the CF surface, contributing to their mechanical interlocking and electrochemical performance. The batteries demonstrate a specific energy density of 62.67 Wh/kg and a specific capacity of 72.7 mAh/g. Furthermore, the cyclic voltammetry experiments reveal the stability of the LFP-CNC-GNP-coated CF batteries over 200 cycles without degradation. This research enables the engineering of hybrid nanostructured battery laminates using novel LFP-CNC-GNP-coated CFs, opening avenues for the development of innovative Li-ion structural batteries. 

Depositing carbon nanotubes (CNTs) into carbon fiber reinforced polymer composites (CFRPs) is challenging because of the need for complicated lab-scale processes and toxic chemical dispersants that makes conventional means of processing less compatible with existing industrial procedures for large-scale applications. In this work, a scalable supercritical CO2-assisted atomization technique is used to effectively deposit hybrid CNTs in CFRPs allowing them to boost their functionality and tailor the microstructure. Cellulose nanocrystals (CNCs) are utilized to create hybrid nanostructures with CNTs (CNC bonded CNT) that enables stabilization of CNTs in nontoxic media, i.e., water, and this promotes the scalability of the process. According to Zeta potential values, CNCs successfully stabilize CNTs in water suspension. Scanning electron microscopy (SEM) micrographs show hybrid CNC bonded CNTs are homogeneously dispersed on the carbon fiber surface. According to the in-situ bending test under the optical microscope, crack propagation is hindered by engineered hybrid CNT nanostructures in the modified CFRP whereas neat CFRP exhibits low crack growth resistance due to the uninterrupted crack propagation in the continuous epoxy matrix. Our results imply that this strategy probes the importance of new controlled manufacturing of hybrid nanostructures through evaporation‑induced self‑assembly of nanocolloidal droplets, and allows for tailoring of the desired properties of nanostructured composites.

 

Cellulose nanocrystal (CNCs) assisted carbon nanotubes (CNTs) and graphene nanoplatelets (GnP) were used to modify the interfacial region of carbon fiber (CF) and polymer matrix to strengthen the properties of carbon fiber-reinforced polymer (CFRP). Before transferring CNC-CNTs and CNC-GnPs on the CF surface by an immersion coating method, the nanomaterials were dispersed in DI water homogeneously by using probe sonication technique without additives. The results showed that the addition of CNC-CNT and CNC-GnP adjusted the interfacial chemistry of CFRP with the formation of polar groups. Furthermore, according to the single fiber fragmentation test (SFFT), the interfacial shear strength (IFSS) of CNC-GnP 6:1 and CNC-CNT 10:1 added CFRP increased to 55 MPa and 64 MPa due to modified interfacial chemistry by the incorporation of the nanomaterials. This processing technique also resulted in improvement in interlaminar shear strength (ILSS) in CFRPs from 35 MPa (neat composite) to 45 (CNC-GnP 6:1) MPa and 52 MPa (CNC-CNT 10:1).