Using molten salts for etching aluminum (Al) away from the MAX phase for MXene synthesis is an attractive alternative method that allows one to avoid the use of toxic hydrofluoric acid (HF) solutions. However, the mechanism of the MAX phase reaction with molten salts remains to date unclear due to the lack of in situ data. Here, we present a detailed in situ time-resolved synchrotron radiation X-ray diffraction study of the MAX phase annealing in molten ZnCl₂ and SnCl₂. The reaction of salts with the MAX phase is found to occur in two stages. The initial period of annealing results in the delamination of two-dimensional (2D) Ti₃C₂ layers, vigorous evolution of AlCl₃ bubbles, and dissolution of Zn in a ZnCl₂ melt. The chlorine-terminated Ti3C2 sheets formed in the delaminated state are restacked into a relatively well-ordered MXene structure (P6₃/mmc, a = 3.071 Å and c = 18.577 Å) during the prolonged annealing in molten salts. Surprisingly, the data recorded directly in molten salts at temperatures up to 873 K demonstrate that Ti₃C₂Cl_x MXene shows no swelling in both liquid ZnCl₂ and SnCl₂. The structure of MXene studied directly in the molten salts is found to be the same as in ex situ experiments performed after cooling and water washing under ambient conditions. The absence of the “pristine” melt-swollen phase indicates a rather different mechanism of MXene formation compared to HF-based solution methods. Formation of MXene by gradually removing Al from the MAX phase starting at the edges of flakes and propagating into the deeper parts of interlayers is not possible, since the molten salt is not capable of penetrating between Cl-terminated Ti₃C₂ layers.

Here, we show that biomass derived from waste wood from forest (silver birch trees, Betula pendula) is an excellent starting material for fabricating activated carbon for supercapacitors. The carbon was prepared via hydrothermal carbonization with H3PO4followed by pyrolysis. The effect of sulfur doping on its physicochemical and electrochemical properties was evaluated. The samples were named BCM (biomass carbon material) for non-doped and S-BCM (sulfur–biomass carbon material) for the doped samples. We further show that sulfur doping (with around 7% sulfur content) radically increases these nanoparticles’ performance, leading to higher capacitance and stability. The sulfur doping increased the specific surface area to 2124 m2g–1compared to non-doped (1972 m2g–1), as reflected in the enhancement of the number of micropores. In addition, according to Raman spectroscopy analysis, the sulfur doping increased the structural defects based on the ID/IGvalues (S-BCM = 2.23 and BCM = 1.98). Furthermore, the sulfur doping increased the hydrophilicity of the carbon particles, allowing us to disperse them in water and use layer-by-layer self-assembly to fabricate supercapacitor electrodes with nanometer-layer precision. The assembled S-BCM electrodes exhibited a higher capacitance than those of pristine carbon with the highest values measured at 79.1 F/g at 1 A/g. They also had higher stability with a capacitance retention of 85.3% after 10 000 charge–discharge cycles. Our work shows a promising route for making advanced high-performance electrode materials for supercapacitors using waste byproducts, which is especially relevant for the Nordic hemisphere, to minimize carbon footprint while enabling advanced energy storage devices as we aim at reach a smooth transition toward a fossil-free future.

Hyperbranched polymers (HBPs) are widely applied nowadays as functional materials for biomedicine needs, nonlinear optics, organic semiconductors, etc. One of the effective and promising ways to synthesize HBPs is a polyaddition of AB2+A2+B4 monomers that is generated in the A2+CB2, AA′+B3, A2+B′B2, and A2+C2+B3 systems or using other approaches. It is clear that all the foundational features of HBPs that are manufactured by a polyaddition reaction are defined by the component composition of the monomer mixture. For this reason, we have designed a structural kinetic model of AB2+A2+B4 monomer mixture polyaddition which makes it possible to predict the impact of the monomer mixture’s composition on the molecular weight characteristics of hyperbranched polymers (number average (DPn) and weight average (DPw) degree of polymerization), as well as the degree of branching (DB) and gel point (pg). The suggested model also considers the possibility of a positive or negative substitution effect during polyaddition. The change in the macromolecule parameters of HBPs formed by polyaddition of AB2+A2+B4 monomers is described as an infinite system of kinetic equations. The solution for the equation system was found using the method of generating functions. The impact of both the component’s composition and the substitution effect during the polyaddition of AB2+A2+B4 monomers on structural and molecular weight HBP characteristics was investigated. The suggested model is fairly versatile; it makes it possible to describe every possible case of polyaddition with various monomer combinations, such as A2+AB2, AB2+B4, AB2, or A2+B4. The influence of each monomer type on the main characteristics of hyperbranched polymers that are obtained by the polyaddition of AB2+A2+B4 monomers has been investigated. Based on the results obtained, an empirical formula was proposed to estimate the pg = pA during the polyaddition of an AB2+A2+B4 monomer mixture: pg = pA = (−0.53([B]0/[A]0)1/2 + 0.78)υAB2 + (1/3)1/2([B]0/[A]0)1/2, where (1/3)1/2([B]0/[A]0)1/2 is the Flory equation for the A2+B4 polyaddition, [A]0 and [B]0 are the A and B group concentration from A2 and B4, respectively, and υAB2 is the mole fraction of the AB2 monomer in the mixture. The equation obtained allows us to accurately predict the pg value, with an AB2 monomer content of up to 80%.

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.

Tunable dynamic networks of cellulose nanofibrils (CNFs) are utilized to prepare high-performance polymer gel electrolytes. By swelling an anisotropically dewatered, but never dried, CNF gel in acidic salt solutions, a highly sparse network is constructed with a fraction of CNFs as low as 0.9%, taking advantage of the very high aspect ratio and the ultra-thin thickness of the CNFs (micrometers long and 2–4 nm thick). These CNF networks expose high interfacial areas and can accommodate massive amounts of the ionic conductive liquid polyethylene glycol-based electrolyte into strong homogeneous gel electrolytes. In addition to the reinforced mechanical properties, the presence of the CNFs simultaneously enhances the ionic conductivity due to their excellent strong water-binding capacity according to computational simulations. This strategy renders the electrolyte a room-temperature ionic conductivity of 0.61 ± 0.12 mS cm−1 which is one of the highest among polymer gel electrolytes. The electrolyte shows superior performances as a separator for lithium iron phosphate half-cells in high specific capacity (161 mAh g−1 at 0.1C), excellent rate capability (5C), and cycling stability (94% capacity retention after 300 cycles at 1C) at 60 °C, as well as stable room temperature cycling performance and considerably improved safety compared with commercial liquid electrolyte systems.

We report a simple and convenient approach to the one-pot synthesis of hyperbranched polyurethane-triazoles with desirable properties. This method is based on in situ generation of an AB(2) + A(2) + B-4 azide-acetylene monomer mixture of known composition, due to quantitative reactions of urethane formation between isophorone diisocyanate (IPDI), 1,3-diazidopropanol-2 (DAPOL) (in the first stage) and propargyl alcohol (in the second stage). The obtained monomer mixture can be involved in step-growth polymerization by azide-alkyne cycloaddition without additional purification (in the third stage). The properties of the resulting polymers should depend on the composition of the monomer mixture. Therefore, first the model revealing the correlation between the monomer composition and the ratio and reactivity of the IPDI and DAPOL active groups is developed and proven. In addition, the newly developed structural kinetic model considering the substitution effect at polyaddition of the complex mixture of monomers allows the prediction of the degree of branching of the target polymer. Based on our calculations, the hyperbranched polyurethane-triazoles were synthesized under found conditions. All products were characterized by H-1 NMR, FTIR, SEC, DLS, DSC, TGA and viscometry methods. It was shown that the degree of branching, molecular weight, intrinsic viscosity, and hydrodynamic radius of the final hyperbranched polymers can be specified at the first stage of one-pot synthesis. The obtained hyperbranched polyurethane-triazoles showed a degree of branching from 0.21 to 0.44 (calculated DB-0.25 and 0.45, respectively).