Lignin has emerged as a sustainable alternative to fossil-based polymers in advanced materials such as photonics. However, current methods for preparing photonic lignin materials are limited by non-benign organic solvents and low production yields. In this work, we present a highly efficient process that enables the production of photonic glasses with yields ranging from 48% to 72%, depending on the size of the lignin nanoparticles obtained from herbaceous soda lignin, softwood kraft lignin, and hardwood organosolv lignin. The hydrodynamic diameter of lignin nanoparticles can be regulated by the rate of water addition to the lignin-ethanol solution. We demonstrate that this control over particle size allows for tailoring the color of the photonic glass across the visible spectrum.

Superinsulating nanofibrillar cellulose foams have the potential to replace fossil-based insulating materials, but the development is hampered by the moisture-dependent heat transport and the lack of direct measurements of phonon transport. Here, inelastic neutron scattering is used together with wide angle X-ray scattering (WAXS) and small angle neutron scattering to relate the moisture-dependent structural modifications to the vibrational dynamics and phonon transport and scattering of cellulose nanofibrils from wood and tunicate, and wood cellulose nanocrystals (W-CNC). The moisture interacted primarily with the disordered regions in nanocellulose, and WAXS showed that the crystallinity and coherence length increased as the moisture content increased. The phonon population derived from directional-dependent phonon density of states (GDOS) increased along the cellulose chains in W-CNC between 5 and 8 wt% D₂O, while the phonon population perpendicular to the chains remained relatively unaffected, suggesting that the effect of increased crystallinity and coherence length on phonon transport is compensated by the moisture-induced swelling of the foam walls. Frequency scaling in the low-energy GDOS showed that materials based on hygroscopic and semicrystalline nanocellulose falls in between the predicted behavior for solids and liquids. Phonon-engineering of hygroscopic biopolymer-based insulation materials is promoted by the insights on the moisture-dependent phonon transport.

Electrochemical energy storage technologies offer means to transition toward a decarbonized society and carbon neutrality by 2050. Compared to conventional lithium-ion batteries, aqueous zinc-ion chemistries do not require scarce materials or toxic and flammable organic-based electrolytes to function, making them favorable contenders in the scenario of intensifying climate change and supply chain crisis. However, environmentally benign and bio-based materials are needed to substitute fossil-based battery materials. Accordingly, this work taps into the possibilities of lignin together with chitosan to form gel polymer electrolytes (GPEs) for zinc-ion chemistries. A simple fabrication process enabling free-standing sodium lignosulfonate–chitosan and micellar lignosulfonate–kraft lignin–chitosan GPEs with diameters exceeding 80 mm is developed. The GPEs combine tensile strength with ductility, reaching Young’s moduli of 55 ± 4 to 940 ± 63 MPa and elongations at break of 14.1 ± 0.2 to 43.9 ± 21.1%. Competitive ionic conductivities ranging from 3.8 to 18.6 mS cm^–1 and electrochemical stability windows of up to +2.2 V vs Zn²⁺/Zn were observed. Given the improved interfacial adhesion of the GPEs with metallic Zn promoted by the anionic groups of the lignosulfonate, a stable cycling of the Zn anode is obtained. As a result, GPEs can operate at 5000 μA cm^–2 with no short-circuit and Coulombic efficiencies above 99.7%, outperforming conventional separator–liquid electrolyte configurations such as the glass microfiber separator soaked into 2 M ZnSO₄ aqueous electrolyte, which short-circuits after 100 μA cm^–2. This work demonstrates the potential of underutilized biorefinery side-streams and marine waste as electrolytes in the battery field, opening new alternatives in the sustainable energy storage landscape beyond LIBs.

The inferior thermoplastic properties have limited production of melt-spun fibers from lignin. Here we report on the controlled esterification of softwood kraft lignin (SKL) to enable scalable, solvent-free melt spinning of microfibers using a cotton candy machine. We found that it is crucial to control the esterification process as melt-spun fibers could be produced from lignin oleate and lignin stearate precursors with degrees of esterification (DE) ranging from 20-50%, but not outside this range. To fabricate a functional hybrid material, we incorporated magnetite nanoparticles (MNPs) into the lignin oleate fibers by melt blending and subsequent melt spinning. Thermogravimetric analysis and X-ray diffraction studies revealed that increasing the weight fraction of MNPs led to improved thermal stability of the fibers. Finally, we demonstrated adsorption of organic dyes, magnetic recovery, and recycling via melt spinning of the regular and magnetic fibers with 95% and 83% retention of the respective adsorption capacities over three adsorption cycles. The mechanical recyclability of the microfibers represents a new paradigm in lignin-based circular materials.

Structural colors in nature have inspired research into engineered photonic materials starting from renewable resources such as lignin extracted from wood and agricultural residues. A notable obstacle in developing lignin-based photonic crystals lies in the use of hazardous organic solvents, giving rise to safety and environmental concerns. Additionally, low product yields hinder scalable production of lignin photonics. Here, we report a highly efficient method for the fabrication of colloidal lignin particles of predicable size for producing photonic crystals using ethanol and water as the sole solvents. We achieved a 78% mass yield of photonic crystals starting from a crude soda lignin, resulting in vibrant colors spanning the entire visible spectrum. Controlling the particle size can be achieved by varying the dilution rate of a lignin ethanol solution with water, enabling the direct generation of colloidal crystals of preferred colors. The new method paves the way for large-scale development of lignin photonics.