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This paper aims to provide a review of four-dimensional (4D) printing of shape memory polymers using inkjet printing technology. 4D printing refers to the three-dimensional (3D) printing of smart materials capable of shape change or function modification with respect to time when activated by external stimuli. Inkjet printing has gained popularity because of the technical advantages such as non-contact deposition, multi-material printing, high resolution, high speed of printing and minimal post processing. This review will serve as a platform for understanding the inkjet 4D printing process and the shape memory capability of the polymer structures printed using inkjet printing.

The approach used in this review was to search for and review research works related to inkjet 4D printing of shape memory polymers. The search period was limited for the duration 2013 to 2021 as the 4D printing technology came into light later in 2013. With the review of inkjet 4D printing of shape memory polymers, the shape memory capability of the inkjet-printed structures were also studied.

With the available research documents, it was found that the inkjet 4D printing technology gained momentum from 2016, three years after the introduction of the 4D printing technology. The key findings of this review show that inkjet 4D printing of shape memory polymers were primarily performed using commercial inkjet printers and polymer inks linked to the printers. Even though the inkjet printing technology is matured enough to print multiple materials, development of shape memory polymer inks for inkjet printability remains complex. To realize the full potential of inkjet 4D printing, novel polymer inks specific for inkjet printing needs development.

The major limitation to this review was the availability of research papers for review. Even though inkjet printing technology has grown to popularity in the graphics printing and publishing industry since its inception in the 19th century, the technology still needs to evolve in the printing of 3D structures due to the limitations in synthesizing inks that are inkjet printable. However, this research will serve as a platform for understating the current status of inkjet 4D printing and the limitations of the technology.

This review focuses only on the inkjet 4D printing of shape memory polymers among the generally summarized 4D printing review papers available. Currently, 4D printing of shape memory polymers is carried out using only the commercially available polymer printers. Also, researchers do not have the flexibility of modifying the polymer inks linked to the printers. This review can spur more research into the development of novel polymer inks specific for inkjet printing.

A review on additive manufacturing (AM) of shape memory polymer composites (SMPCs) is put forward to highlight the progress made up to date, conduct a critical review and show the limitations and possible improvements in the different research areas within the different AM techniques. The purpose of this study is to identify academic and industrial opportunities.

This paper introduces the reader to three-dimensional (3 D) and four-dimensional printing of shape memory polymers (SMPs). Specifically, this review centres on manufacturing technologies based on material extrusion, photopolymerization, powder-based and lamination manufacturing processes. AM of SMPC was classified according to the nature of the filler material: particle dispersed, i.e. carbon, metallic and ceramic and long fibre reinforced materials, i.e. carbon fibres. This paper makes a distinction for multi-material printing with SMPs, as multi-functionality and exciting applications can be proposed through this method. Manufacturing strategies and technologies for SMPC are addressed in this review and opportunities in the research are highlighted.

This paper denotes the existing limitations in the current AM technologies and proposes several directions that will contribute to better use and improvements in the production of additive manufactured SMPC. With advances in AM technologies, gradient changes in material properties can open diverse applications of SMPC. Because of multi-material printing, co-manufacturing sensors to 3D printed smart structures can bring this technology a step closer to obtain full control of the shape memory effect and its characteristics. This paper discusses the novel developments in device and functional part design using SMPC, which should be aided with simple first stage design models followed by complex simulations for iterative and optimized design. A change in paradigm for designing complex structures is still to be made from engineers to exploit the full potential of additive manufactured SMPC structures.

Advances in AM have opened the gateway to the potential design and fabrication of functional parts with SMPs and their composites. There have been many publications and reviews conducted in this area; yet, many mainly focus on SMPs and reserve a small section to SMPC. This paper presents a comprehensive review directed solely on the AM of SMPC while highlighting the research opportunities.

The purpose of this paper is to provide a review of recent systematic and comprehensive advancement in electrospun polymer fiber and their composites with shape memory property.

The nanofiber manufacture technique is initially reviewed. Then, the influence of electrospinning parameters and actuation method has been discussed. Finally, the study concludes with a brief review of recent development in potential applications.

Shape memory polymer (SMP) nanofibers are a type of smart materials which can change shape under external stimuli (e.g. temperature, electricity, magnetism, solvent). In general, such SMP nanofibers could be easily fabricated by mature electrospinning technique. The nanofiber morphology is mainly affected by the electrospinning parameters, including applied voltage, tip-to-collector distance, viscosity of solution, humidity and molecular weight. For actuation method, most SMP nanofibers and their composites can change their shapes in response to heat, magnetic field or solvent, while few can be driven by electricity. Compared with the block SMPs, electrospun SMP nanofibers’ mat with porosity and low mechanical property have a wide potential application field including tissue engineering, drug delivery, filtration, catalysis.

This paper provides a detailed review of shape memory nanofibers: fabrication, actuation and potential application, in the near future.

The purpose of this paper is to study the influence of calcium sulfate whiskers (CSWs) on the thermodynamic properties and shape memory properties of epoxy/cyanate ester shape memory composites.

To improve the mechanical properties of shape memory cyanate ester (CE)/epoxy polymer (EP) resin, high performance CSWs were used to reinforce the thermo-induced shape memory CE/EP composites and the shape memory CSW/CE/EP composites were prepared by molding. The effect of CSW on the mechanical properties and shape memory behavior of shape memory CE/EP composites was investigated.

After CSW filled the shape memory CE/EP composites, the bending strength of the composites is greatly improved. When the content of CSW is 5 Wt.%, the bending strength of the composite is 107 MPa and the bending strength is increased by 29 per cent compared with bulk CE/EP resin. The glass transition temperature and storage modulus of the composites were improved in CE/EP resin curing system. However, when the content of CSW is more than 10 Wt.%, clusters are easily formed between whiskers and the voids between whiskers and matrix increase, which will lead to the decrease of mechanical properties of composites. The results of shape memory test show that the shape memory recovery time of the composites decreases with the decrease of CSW content at the same temperature. In addition, the shape recovery ratio of the composites decreased slightly with the increase of the number of thermo-induced shape memory cycles.

A simple way for fabricating thermo-activated SMP composites has been developed by using CSW.

The outcome of this study will help to fabricate the SMP composites with high mechanical properties and the shape memory CSW/CE/EP composites are expected to be used in space deployable structures.

The purpose of this paper is to understand the recovery mechanism of poly(trimethylene terephthalate) (PTT) shape memory fabrics.

Tests were designed to study the effects of force, temperature and their combinations on the fabrics' crease recoveries. In the test a cantilever device and an ironing force which simulated people ironing their clothes were used, respectively.

Temperature was found to have little effect on the recovery of both the warp and filling of the fabrics. Crease recoveries did not improve significantly when the temperature was increased to above the polymer's glass transition. However, forces, applied in primarily compressive and tensile modes to simulate ironing and hand stroking actions, were found to be very effective in the fabrics' crease recoveries. Recoveries were 81‐87 per cent even when the applied force was very small, at 5 N/cm². When forces were applied at elevated temperatures, just below and above the polymer's glass transition, there were no significant improvements in crease recoveries. Therefore, force was the main factor in PTT shape memory fabrics' recovery mechanism for the fabrics to return to their initial shapes.

The results suggest that PTT shape memory fabric has excellent shape recoverability and easy care property and it has large application potentiality.

This paper aims to focus on achieving triple-shape memory effect (triple-SME) of a commercial poly (ethylene terephthalate) (PET) film with the thickness of 100 µm.

The thermal characteristics and microstructure of PET film were characterized by differential scanning calorimetry, thermogravimetric analysis and wide-angle X-ray diffraction analysis. The dual-shape memory effect (dual-SME) of the PET film was then systematically investigated, and based on that, triple-SME in thin PET film was achieved.

Investigation of the dual-SME in PET film revealed the difference between recovery temperature and programming temperature reduced with increasing programming temperature. An obvious intermediate shape shifting between the original and final programmed shape was observed during shape recovery in triple-shape memory behaviors.

Compared with dual-SME in polymer, relatively less work has been done on multi-SME in polymer, especially in thin polymer film. In this study, triple-SME in a PET film was investigated based on the results of dual-SME of the film. The main implication of the study is on how to achieve a watermark between the final programmed pattern and the original pattern, for the application of shape memory polymer in anti-counterfeiting label.

Dual- and triple-SMEs were achieved in a PET film that is only 100 µm in thickness, and the underlying mechanism for the difference between programming temperature and recovery temperature was discussed. For the novel application of triple-SME in anti-counterfeit label, the watermark during shape recovery in triple-SME can effectively prevent duplication.

This study aims to present that the chemo-responsive shape recovery of thermoplastic polyurethane (TPU) is tunable by solvents with different solubility parameters, and it is generic for chemo-responsive shape-memory polymer and its composites.

Two kinds of commercial TPU samples with different thicknesses were prepared by panel vulcanizer and injection molding (an industrial manner) to investigate their chemo-responsive shape memory properties in acetic ether and acetone.

Results showed that all of TPU films with different thicknesses can fully recover their original shapes weather they recover in acetic ether or acetone. But the recovery time of TPU films in acetone is greatly reduced, especially for the twisting samples. The residual strains of recovery TPU samples after extension reduce obviously.

The great decrement of recovery time is related to two factors. One is due to the bigger solubility parameter of acetone with higher dipole moment compared with those of acetic ether, and the other is the remained internal stress of TPU films after preparation. The internal stress is identified to have an effect on the shape-memory properties by comparing the recovery process of samples with/without annealing. The reduced residual strains of recovery TPU samples after extension is due to the increasing mobility of polymer segments after molecules of acetic ether penetrates into the polymeric chains.

This is a universal strategy to control the recovery process of shape-memory materials or composites. The underlying mechanism is generic and should be applicable to chemo-responsive shape-memory polymers or their composites.

Shape memory materials are functional materials having a good number of applications due to their unique features of programmable material technology such as self-stretching, self-assembly and self-tightening. Advancements in today’s technology led to the easy fabrication of such novel materials using 3D printing techniques. When an external stimulus causes a 3D printed specimen to change shape on its own, this process is known as 4D printing. This study aims to investigate the effect of graphene nano platelet (GNPs) on the shape memory behaviour of shape memory photo polymer composites (SMPPCs) and to optimize the shape-changing response by using the Taguchi method.

SMPPCs are synthesized by blending different weight fractions (Wt.%) of flexible or soft photopolymer (FPP) resin with hard photopolymer (HPP) resin, then reinforced with GNPs at various Wt.% to the blended PP resin, and then fabricated using masked stereolithography (MSLA) apparatus. The shape memory test is conducted to assess the shape recovery time (T), shape fixity ratio (R_f), shape recovery ratio (R_r) and shape recovery rate (V_r) using Taguchi analysis by constructing an L9 orthogonal array with parameters such as Wt.% of a blend of FPP and HPP resin, Wt.% of GNPs and holding time.

SMPPCs with A3, B3 and C2 result in a faster T with 2 s, whereas SMPPCs with A1, B1 and C3 result in a longer T with 21 s. The factors A and B are ranked as the most significant in the Pareto charts that were obtained, whereas C is not significant. It can be seen from the heatmap plot that when factors A and B increase, T is decreasing and V_r is increasing. The optimum parameters for T and V_r are A3, B3 and C2 at the same time for R_f and R_r are A1, B3 and C1.

Faster shape recovery results from a higher Wt.% of FPP resin in a blend than over a true HPP resin. This is because the flexible polymer links in FPP resin activate more quickly over time. However, a minimum amount of HPP resin also needs to be maintained because it plays a role in producing higher R_f and V_r. The use of GNPs as reinforcement accelerates the T because nanographene conducts heat more quickly, releasing the temporary shape of the specimen more quickly.

The use of FPP and HPP resin blends, fabricating the 4D-printed SMPPCs specimens with MSLA technology, investigating the effect of GNPs and optimizing the process parameters using Taguchi and the work was validated using confirmation tests and regression analysis, which increases the originality and novelty.

This article aims to present a systematic and up-to-date account of carbon-based reinforcements, including carbon nanotube (CNT), carbon nanofibre (CNF), carbon black (CB), carbon fibre (CF) and grapheme, in shape-memory polymer (SMP) for electrical actuation.

Studies exploring carbon-based reinforcement in SMP composites for electrically conductive performance and Joule heating triggered shape recovery have been included, especially for the principle design, characterisation and shape recovery behaviour, making the article a comprehensive account of the systemic progress in SMP composite incorporating conductive carbon reinforcement.

SMPs are fascinating materials and have attracted great academic and industrial attention owing to their significant macroscopic shape deformation in the presence of an appropriate stimulus. The working mechanisms, the physico requirements and the theoretical origins of the different types of carbon-based reinforcement SMP composites have been discussed. Current research and development on the fabrication strategies of carbon-based reinforcement SMP composites have been summarised.

A systematic review is to evaluate carbon-based reinforcements in SMPs for electrical actuation and discuss recent developments and future applications.

Carbon-based reinforcements in SMPs can be used as smart deployable space structure in the broad field of aerospace technologies.

To reveal the research and development of utilising CNT, CNF, CB, CF and grapheme to achieve shape recovery of SMP composites through electrically resistive heating, which will significantly benefit the research and development of smart materials and systems.

Epoxy (EP) and polye-caprolactone (PCL) are typical dual-shape memory polymer (DSMP). To get excellent triple-shape memory effect (TSME) polymer composites which are made from EP and PCL. Miscible PCL/EP blend composites have been investigated and compared to the TSMEs with electrospun PCL microfiber membranes/EP composites. Clay montmorillonite (MMT)-modified electrospun PCL microfiber membranes were prepared to improve the shape memory fixities of electrospun PCL microfiber membranes/EP composites.

The morphologies of electrospun PCL microfiber membranes and the cross section of PCL/EP composites were studied using a field emission scanning electron microscope (FE-SEM), and the existence of MMT was confirmed by a transmission electron microscope. Thermal mechanical properties were observed by a differential scanning calorimeter (DSC) and a dynamic thermomechanical analysis machine, and the TSMEs were also determined through dynamic mechanical analysis.

Results indicate that the TSMEs of electrospun PCL microfiber membranes/EP composites were excellent, whereas the TSMEs of PCL/EP blend composites were poor. The TSMEs of PCL electrospun microfiber membranes/EP composites significantly improved with the addition of the PCL electrospun microfiber modified with moderate MMT.

Adding a moderate content of MMT into the electrospun PCL fibers, could improve the TSME of the PCL fiber membranes/EP composites. This study was to create a simple and effective method that can be applied to improve the performance of other SMP.

A novel triple-shape memory composite were made from dual-shape memory EP and electrospun PCL fiber membranes.