Paper is the largest renewable industrial substrate produced for various applications and can be recycled by disintegrating the fibers and reforming the paper. Paper and its fiber constituents lack functions such as electrical conductivity and papermaking itself has not been used for producing electronic devices. In this work, we show a potential industrially viable route for introducing cationic charges on the cellulose fibers and subsequently show how the adsorption of negatively charged ionically and electrically conductive materials onto these fibers from aqueous media can be applied at time scales relevant to industrial papermaking. This results in electroactive fibers, that can subsequently be used to prepare electroactive papers using standard papermaking procedures. Since fibers in the paper can selectively be coated with different active materials, various functions can be added into the paper. To demonstrate applications, we prepared electroactive papers using fibers with adsorbed carbon nanotubes (CNTs) and conducting polymers. We achieved conductivity of 21 S/m with only 1wt% CNT. We also prepared papers with CNTs and black phosphorus, used as paper-based lithium, and sodium ion battery (free-standing) anodes. They delivered a specific capacity of 642 mA h g⁻¹ at 100 mA g⁻¹ after 3500 cycles with 99.5% columbic efficiency. Furthermore, we recycled the papers, and as the disintegration of the fibers did not lead to removal of the ionic or electroactive materials from the fiber surface, the recycled papers showed similar electrical and mechanical properties to the original papers. This opens the path for recyclable paper-based electronics.

The unique properties of hydrogels enable the design of life-like soft intelligent systems. However, stimuli-responsive hydrogels still suffer from limited actuation control. Direct electronic control of electronically conductive hydrogels can solve this challenge and allow direct integration with modern electronic systems. An electrochemically controlled nanowire composite hydrogel with high in-plane conductivity that stimulates a uniaxial electrochemical osmotic expansion is demonstrated. This materials system allows precisely controlled shape-morphing at only −1 V, where capacitive charging of the hydrogel bulk leads to a large uniaxial expansion of up to 300%, caused by the ingress of ≈700 water molecules per electron–ion pair. The material retains its state when turned off, which is ideal for electrotunable membranes as the inherent coupling between the expansion and mesoporosity enables electronic control of permeability for adaptive separation, fractionation, and distribution. Used as electrochemical osmotic hydrogel actuators, they achieve an electroactive pressure of up to 0.7 MPa (1.4 MPa vs dry) and a work density of ≈150 kJ m−3 (2 MJ m−3 vs dry). This new materials system paves the way to integrate actuation, sensing, and controlled permeation into advanced soft intelligent systems.

This work presents a route to fabricate micropatterned conductive structures where the conductors are monolithically integrated with nanocellulose-based paper. To fabricate conductive features, microstructures are patterned on filter papers using wax-printing, followed by vacuum filtration of carbon nanotubes (CNTs) or silver nanowires (AgNWs) dispersed in aqueous cellulose nanofibrils (CNFs). These patterns are then laminated onto a pure CNF substrate (both in gel-state) and dried to form cellulose nanopapers with integrated conductive micropatterns. Resolutions of the conductive features are shown down to 400 µm wide, 250 nm thick, and with conductivity values of 115 ± 5 S cm −1 for the CNF–CNT and 3770 ± 230 S cm −1 for the CNF–AgNW micropatterns. The nanopaper and the conductive patterns both constitute random fibrous networks, and they display similar ductility and swelling behavior in water. Thus, the integrated conductive micropatterns can withstand folding, as well as wetting cycles. This stability of the micropatterns makes them useful in various devices based on nanocellulose substrates. As an example, an electroanalytical nanopaper device that operates in wet conditions is demonstrated.

Perovskite solar cells (PSCs) has skyrocketed in the past decade to an unprecedented level due to their outstanding photoelectric properties and facile processability. However, the utilization of expensive hole transport materials (HTMs) and the inevitable instability instigated by the deliquescent dopants represent major concerns hindering further commercialization. Here, a series of low-cost, conjugated polymers are designed and applied as dopant-free HTMs in PSCs, featuring tuned energy levels, good temperature and humidity resistivity, and excellent photoelectric properties. Further studies highlight the critical and multifaceted roles of the polymers with respect to facilitating charge separation, passivating the surface trap sites of perovskite materials, and guaranteeing long-term stability of the devices. A stabilized power conversion efficiency (PCE) of 20.3% and remarkably enhanced device longevity are achieved using the dopant-free polymer P3 with a low concentration of 5 mg/mL, qualifying the device as one of the best PSC systems constructed on the basis of dopant-free HTMs so far. In addition, the flexible PSCs based on P3 also exhibit a PCE of 16.2%. This work demonstrates a promising route toward commercially viable, stable, and efficient PSCs.

Perovskite photovoltaics have recently attracted extensive attention due to their unprecedented high power conversion efficiencies (PCEs) in combination with primitive manufacturing conditions. However, the inherent polycrystalline nature of perovskite films renders an exceptional density of structural defects, especially at the grain boundaries (GBs) and film surfaces, representing a key challenge that impedes the further performance improvement of perovskite solar cells (PSCs) and large solar module ambitions towards commercialization. Here, a novel strategy is presented utilizing a simple ethylammonium chloride (EACl) additive in combination with a facile solvent bathing approach to achieve high quality methyammonium lead iodide (MAPbI3) films. Well-oriented, micron-sized grains were observed, which contribute to an extended carrier lifetime and reduced trap density. Further investigations unraveled the distinctively prominent effects of EACl in modulating the perovskite film quality. The EACl was found to promote the perovskite grain growing without undergoing the formation of intermediate phases. Moreover, the EACl was also revealed to deplete at relative low temperature to enhance the film quality without compromising the beneficial bandgap for solar cell applications. This new strategy boosts the power conversion efficiency (PCE) to 20.9% and 19.0% for devices with effective areas of 0.126 cm2 and 1.020 cm2, respectively, with negligible current hysteresis and enhanced stability. Besides, perovskite films with a size of 10 × 10 cm2, and an assembled 16 cm2(5 × 5 cm2 module) perovskite solar module with a PCE of over 11% were constructed.

The mechanical properties of cellulose nanofibrils network structure are essential for their applications in functional materials. In this work, an adhesive peptide consisting of just 11 amino acid residues with a hydrophobic core sequence of FLIVI (F – phenylalanine, L – leucine, I – isoleucine, V – valine) flanked by three lysine (K) residues was adsorbed to 2,2,6,6-Tetramethyl-1-piperidinyloxy radical (TEMPO) oxidized cellulose nanofibrils (TO-CNF). Composite films were prepared by solution casting from water suspensions of TO-CNF adsorbed with the adhesive peptide. The nanofibrils network structure of the composite was characterized by atomic force microscopy (AFM). The structure of the peptide in the composites and the interactions between TO-CNF and the peptide were studied by Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD). The mechanical properties of the composites were characterized by tensile tests and dynamic mechanical analysis (DMA). With 6.3 wt.% adhesive peptide adsorbed onto TO-CNF, the composite showed a modulus of 12.5 ± 1.4 GPa, a tensile strength of 344.5 ± (15.3) MPa, and a strain to failure of 7.8 ± 0.4%, which are 34.4%, 48.8%, and 23.8% higher than those for neat TO-CNF, respectively. This resulted in significantly improved toughness (work to fracture) for the composite, 77% higher than that for the neat TO-CNF.

Deformation mechanisms are largely unknown for superelastic carbon nanotube (CNT) aerogels, and this hampers materials design efforts. The CNT network in the cell walls is typically crosslinked or connected by a thermoset polymer phase. In order to create a recyclable superelastic aerogel, unmodified single or multi-walled CNTs were dispersed in water by adding to aqueous carboxymethyl cellulose (CMC) solution. Directional freeze-drying was used to form honeycombs with cell walls of random-in-the-plane CNTs in CMC matrix. Cell wall morphology and porosity were studied and related to CNT type and content, as well as elastic or plastic buckling of the cell walls under deformation. CMC acts as a physical crosslinker for the CNTs in a porous cell wall. Aerogel structure and properties were characterized before and after recycling. The conductivity of the composite aerogel with a density of 10 kg/m³, 99% porosity and 50 wt % single-walled CNT exceeds 0.5 S/cm. The potential of these superelastic and conductive aerogels for applications such as mechanoresponsive materials was examined in cyclic conductivity tests at different strains. This opens a new route for recyclable superelastic CNT composite aerogels, avoiding material loss, chemical treatment or addition of other components.

A perylenediimide (PDI) tetramer-based three dimensional (3D) molecular material, termed SFX-PDI4, has been designed, synthesized, and characterized. The low-lying HOMO and LUMO energy levels, high electron mobility and good film-formation property make it a promising electron transport material (ETM) in inverted planar perovskite solar cells (PSCs). The device exhibits a high power conversion efficiency (PCE) of 15.3% with negligible hysteresis, which can rival that of device based on PC61BM. These results demonstrate that three dimensional PDI-based molecular materials could serve as high performance ETMs in PSCs.

Non-leaking, green materials with high content of phase change materials (PCM) can conserve solar energy and contribute to a sustainable society. Here, paraffin was encapsulated by nanocellulose (CNF) through a pickering emulsion method, while simultaneously forming a composite material. The thermodynamic drive for phase separation was confirmed by molecular modeling. Particle formation was characterized by dynamic light scattering and they were processed into stable PCM/CNF composites in the form of PCM paper structures with favorable mechanical properties. The PCM composite was lightweight and showed a solid content of paraffin of more than 72 wt%. Morphology was characterized using FE-SEM. The thermal regulation function of the PCM composite was demonstrated in the form of a model roof under simulated sunlight. No obvious leakage was observed during heating/cooling cycles, as supported by DSC and SAXS data. The PCM composite can be extended to panels used in energy-efficient smart buildings with thermal regulation integrated in load-bearing structures.