Most products today have several functions, but these are achieved by integrating different monofunctional devices and/or materials in a system. Having several functions simultaneously in one single material has many potential advantages, such as a structural material that can also store energy, have self-sensing or self-healing capability or any other physical function. This would lead mass and resource savings, being more energy efficient and thus more sustainable. This paper presents a mini review on how carbon fibres can be used for integrating several functions simultaneously in a high-performance load carrying structural material using the electrical and electrochemical properties of carbon fibres. Through this carbon fibre composites can also store energy like a lithium-ion battery, be used as a strain sensor, have electrically controlled actuation and shape-morphing, and be used as an energy harvester.

Multifunctional structural materials are capable of reducing system level mass and increasing efficiency in load -carrying structures. Materials that are capable of harvesting energy from the surrounding environment are advantageous for autono-mous electrically powered systems. However, most energy harvesting materials are non-structural and add parasitic mass, reducing structural efficiency. Here, we show a structural energy harvesting composite material consisting of two carbon fiber (CF) layers embedded in a structural battery electrolyte (SBE) with a longitudinal modulus of 100 GPa-almost on par with commercial CF pre-pregs. Energy is harvested through mechanical deforma-tions using the piezo-electrochemical transducer (PECT) effect in lithiated CFs. The PECT effect creates a voltage difference between the two CF layers, driving a current when deformed. A specific power output of 18 nW/g is achieved. The PECT effect in the lithiated CFs is observed in tension and compression and can be used for strain sensing, enabling structural health monitoring with low added mass. The same material has previously been shown capable of shape morphing. The two additional functionalities presented here result in a material capable of four functions, further demonstrating the diverse possibilities for CF/SBE composites in multifunctional applications in the future.

Engineering materials that can store electrical energy in structural load paths can revolutionize lightweight design across transport modes. Stiff and strong batteries that use solid-state electrolytes and resilient electrodes and separators are generally lacking. Herein, a structural battery composite with unprecedented multifunctional performance is demonstrated, featuring an energy density of 24 Wh kg−1 and an elastic modulus of 25 GPa and tensile strength exceeding 300 MPa. The structural battery is made from multifunctional constituents, where reinforcing carbon fibers (CFs) act as electrode and current collector. A structural electrolyte is used for load transfer and ion transport and a glass fiber fabric separates the CF electrode from an aluminum foil-supported lithium–iron–phosphate positive electrode. Equipped with these materials, lighter electrical cars, aircraft, and consumer goods can be pursued.

By increasing the number of functions a structure performs it is possible to save weight and volume on a systems level. Ion-insertion in carbon fibres (CFs) is a way to create multifunctional structures for energy storage, morphing, and strain-sensing. Previous studies have focussed on lithium- and sodium-insertion to create multifunctionality. However, with a larger ionic radius and a chemistry more amenable to insertion in polyacrylonitrile (PAN)-based CFs, potassium-insertion is a promising way forward. Here, a study is conducted to examine potassium-insertion in intermediate modulus PAN-based CFs for multifunctionality. Electrochemical cycling shows a maximum reversible capacity of 170 mAh/g, with ex-situ mechanical testing showing a small impact on the CFs’ mechanical properties post-cycling. Operando measurements show a maximum reversible CF expansion during potassium-insertion of 0.24%, and analytical modelling illustrates that such strains can generate significant deformations in a morphing structure. A voltage-strain coupling of 0.26 V/unit strain is also found. Results are compared with previous work on lithium- and sodium-insertion, with the conclusion that potassium-insertion is more promising than sodium-insertion, but less so than lithium-insertion for multifunctional structures.

Structures that are capable of changing shape can increase efficiency in many applications, but are often heavy and maintenance intensive. To reduce the mass and mechanical complexity solid-state morphing materials are desirable but are typically nonstructural and problematic to control. Here we present an electrically controlled solid-state morphing composite material that is lightweight and has a stiffness higher than aluminum. It is capable of producing large deformations and holding them with no additional power, albeit at low rates. The material is manufactured from commercial carbon fibers and a structural battery electrolyte, and uses lithium-ion insertion to produce shape changes at low voltages. A proof-of-concept material in a cantilever setup is used to show morphing, and analytical modeling shows good correlation with experimental observations. The concept presented shows considerable promise and paves the way for stiff, solid-state morphing materials.

Morphing structures have long been desired in the various industries to enable, for example, efficient fluid flow in different flow regimes. However, problems with mechanical complexity, weight,

and large energy requirements have meant that morphing structures have only been sparingly utilised. Current state of the art morphing technologies use systems of mechanical motors and hydraulics to create shape changes. These systems add parasitic weight, and are mechanically complex, adding to maintenance costs. Attempts have been made to use solid-state devices such as piezo-ceramics and shape memory alloys to create shape changes, however these devices rely on either extremely high voltages, or changes in atmospheric conditions in order to actuate. They also have comparatively poor mechanical properties. Here we present a concept of a solid-state electrochemically-actuated morphing structure manufactured from aerospace grade carbon fibre. The concept exploits expansions caused by lithium-ions intercalating into the carbon fibre microstructure. Both analytical and FE models are used to simulate a morphing three-layer laminate in a cantilever setup, and it is shown that relatively large deflections could be achieved, albeit at relatively low frequencies (in the range of mHz). An analysis of the likelihood of delamination occurring showed that there are no layups for which delamination is likely based on the estimated interlaminar strengths, and it is therefore unlikely that such a device would suffer from delamination in normal operational conditions. This concept paves the way for a new type of morphing structure that is mechanically simple, lightweight, and uses a low amount of energy to produce large shape changes without loss of mechanical integrity.

Carbon fibres (CFs), originally made for use in structural composites, have also been demonstrated as high capacity Li-ion battery negative electrodes. Consequently, CFs can be used as structural electrodes; simultaneously carrying mechanical load and storing electrical energy in multifunctional structural batteries. To date, all CF microstructural designs have been generated to realise a targeted mechanical property, e.g. high strength or stiffness, based on a profound understanding of the relationship between the graphitic microstructure and the mechanical performance. Here we further advance this understanding by linking CF microstructure to the lithium insertion mechanism and the resulting electrochemical capacity. Different PAN-based CFs ranging from intermediate-to highmodulus types with distinct differences in microstructure are characterised in detail by SEM and HRTEMand electrochemical methods. Furthermore, the mechanism of Li-ion intercalation during charge/discharge is studied by in situ confocal Raman spectroscopy on individual CFs. RamanGband analysis reveals a Li-ion intercalation mechanism in the high-modulus fibre reminiscent of that in crystalline graphite. Also, the combination of a relatively low capacity of the high-modulus CFs (ca. 150 mAh g-1) is shown to be due to that the formation of a staged structure is frustrated by an obstructive turbostratic disorder. In contrast, intermediate-modulus CFs, which have significantly higher capacities (ca. 300 mAh g-1), have Raman spectra indicating a Li-ion insertion mechanism closer to that of partly disordered carbons. Based on these findings, CFs with improved multifunctional performance can be realised by tailoring the graphitic order and crystallite sizes.

An investigation is conducted into the potential for sodiated PAN-based carbon fibers (CFs) to be used in multifunctional actuation, sensing, and energy harvesting. Axial CF expansion/contraction is measured during sodiation/desodiation using operando strain measurements. The reversible expansion/contraction is found to be 0.1% - which is lower than that of lithiated CFs. The axial sodiation expansion occurs in two well-defined stages, corresponding to the sloping and plateau regions of the galvanostatic cycling curve. The results indicate that the sloping region most likely corresponds to sodium insertion between graphitic sheets, while the plateau region corresponds to sodium insertion in micropores. A voltage-strain coupling is found for the CFs, with a maximum coupling factor of 0.15 +/- 0.01 V/unit strain, which could be used for strain sensing in multifunctional structures. This voltage-strain coupling is too small to be exploited for harvesting mechanical energy. The measured axial expansion is further used to estimate the capacity loss due to solid electrolyte interphase (SEI) formation, as well as capacity loss due to sodium trapped in the CF microstructure. The outcomes of this research suggest that sodiated CFs show some potential for use as actuators and sensors in future multifunctional structures, but that lithiated CFs show more promise.

In order to aid design of future structural battery components an analytical model is developed for modelling volume expansions in laminated structural batteries. Volume expansions are caused by lithium ion intercalation in carbon fibre electrodes. An extended version of Classical Lamination Plate Theory (CLPT) is used to allow analysis of unbalanced and unsymmetric lay-ups. The fibre intercalation expansions are treated analogously to a thermal problem, based on experimental data, with intercalation coefficients relating the fibre capacity linearly to its expansions. The model is validated using FEM and allows the study of the magnitude of interlaminar stresses and hence the risk of delamination damage due to the electrochemically induced expansions. It also enables global laminate deformations to be studied. This allows information about favourable lay-ups and fibre orientations that minimise deformations and the risk of delamination to be obtained. Favourable configurations for application to a solid state mechanical actuator are also given.

Multifunctional structural materials are capable of reducing systems-level mass and increasing efficiency in load-carrying structures. Materials that are capable of harvesting energy from the surrounding environment are advantageous for autonomous electrically powered systems. However, most energy harvesting materials are non-structural and add parasitic mass, reducing structural efficiency. Here we show a structural energy harvesting composite material consisting of two carbon fibre (CF) layers embedded in a structural battery electrolyte (SBE) with a longitudinal modulus of 100 GPa – almost on par with commercial carbon fibre pre-pregs. Energy is harvested through mechanical deformations using the piezo- electrochemical transducer (PECT) effect in lithiated CFs. The PECT effect creates a voltage difference between the two CF layers, driving a current when deformed. A specific power output of 18 nW/g is achieved. The PECT effect in the lithiated CFs is observed in tension and compression, and can be used for strain-sensing, enabling structural health monitoring with low added mass. The same material has previously been shown capable of shape- morphing. The two additional functionalities presented here result in a material capable of four functions, further demonstrating the diverse possibilities for CF/SBE composites in multifunctional applications in the future.