Kraft lignin, a by‐product from the production of pulp, is currently incinerated in the recovery boiler during the chemical recovery cycle, generating valuable bioenergy and recycling inorganic chemicals to the pulping process operation. Removing lignin from the black liquor or its gasification lowers the recovery boiler load enabling increased pulp production. During the past ten years, lignin separation technologies have emerged and the interest of the research community to valorize this underutilized resource has been invigorated. The aim of this Review is to give (1) a dedicated overview of the kraft process with a focus on the lignin, (2) an overview of applications that are being developed, and (3) a techno‐economic and life cycle asseeements of value chains from black liquor to different products. Overall, it is anticipated that this effort will inspire further work for developing and using kraft lignin as a commodity raw material for new applications undeniably promoting pivotal global sustainability concerns.

This review is focused on assessment of solvents for cellulose dissolution and the mechanism of regeneration of the dissolved biopolymer. The solvents of interest are imidazole-based ionic liquids, quaternary ammonium electrolytes, salts of super-bases, and their binary mixtures with molecular solvents. We briefly discuss the mechanism of cellulose dissolution and address the strategies for assessing solvent efficiency, as inferred from its physico-chemical properties. In addition to the favorable effect of lower cellulose solution rheology, microscopic solvent/solution properties, including empirical polarity, Lewis acidity, Lewis basicity, and dipolarity/polarizability are determinants of cellulose dissolution. We discuss how these microscopic properties are calculated from the UV-Vis spectra of solvatochromic probes, and their use to explain the observed solvent efficiency order. We dwell briefly on use of other techniques, in particular NMR and theoretical calculations for the same purpose. Once dissolved, cellulose is either regenerated in different physical shapes, or derivatized under homogeneous conditions. We discuss the mechanism of, and the steps involved in cellulose regeneration, via formation of mini-sheets, association into “mini-crystals”, and convergence into larger crystalline and amorphous regions. We discuss the use of different techniques, including FTIR, X-ray diffraction, and theoretical calculations to probe the forces involved in cellulose regeneration.

There is a sustained interest in developing solvents for physically dissolving cellulose, i.e., without covalent bond formation. The use of ionic liquids, ILs, has generated much interest because of their structural versatility that results in efficiency as cellulose solvents. Despite some limitations, imidazole-based ILs have received most of the scientific community’s attention. The objective of the present review is to show the advantages of using quaternary ammonium electrolytes, QAEs, including salts of super bases, as solvents for cellulose dissolution, shaping, and derivatization, and as a result, increase the interest in further investigation of these important solvents. QAEs share with ILs structural versatility; many are liquids at room temperature or are soluble in water and molecular solvents (MSs), in particular dimethyl sulfoxide. In this review we first give a historical background on the use of QAEs in cellulose chemistry, and then discuss the common, relatively simple strategies for their synthesis. We discuss the mechanism of cellulose dissolution by QAEs, neat or as solutions in MSs and water, with emphasis on the relevance to cellulose dissolution efficiency of the charge and structure of the cation and. We then discuss the use of cellulose solutions in these solvents for its derivatization under homogeneous and heterogeneous conditions. The products of interest are cellulose esters and ethers; our emphasis is on the role of solvent and possible side reactions. The final part is concerned with the use of cellulose dopes in these solvents for its shaping as fibers, a field with potential commercial application.

Material recycling requires solutions that are technically, as well as economically and ecologically, viable. In this work, the technical feasibility to separate textile blends of viscose and polyester using alkaline hydrolysis is demonstrated. Polyester is depolymerized into the monomer terephthalic acid at high yields, while viscose is recovered in a polymeric form. After the alkaline treatment, the intrinsic viscosity of cellulose is decreased by up to 35%, which means it may not be suitable for conventional fiber-to-fiber recycling; however, it might be attractive in other technologies, such as emerging fiber processes, or as raw material for sugar platforms. Further, we present an upscaled industrial process layout, which is used to pinpoint the areas of the proposed process that require further optimization. The NaOH economy is identified as the key to an economically viable process, and several recommendations are given to decrease the consumption of NaOH. To further enhance the ecological end economic feasibility of the process, an increased hydrolysis rate and integration with a pulp mill are suggested.

Chemical recycling of textiles holds the potential to yield materials of equal quality and value as products from virgin feedstock. Selective depolymerization of textile polyester (PET) from regenerated cellulose/PET blends, by means of alkaline hydrolysis, renders the monomers of PET while cellulose remains in fiber form. Here, we present the mechanism and reactivity of textile PET during alkaline hydrolysis. Part I of this article series focuses on the cellulose part and a possible industrialization of such a process. The kinetics and reaction mechanism for alkaline hydrolysis of polyester packaging materials or virgin bulk polyester are well described in the scientific literature; however, information on depolymerization of PET from textiles is sparse. We find that the reaction rate of hydrolysis is not affected by disintegrating the fabric to increase its surface area. We ascribe this to the yarn structure, where texturing and a low density assures a high accessibility even without disintegration. The reaction, similar to bulk polyester, is shown to be surface specific and proceeds via endwise peeling. Finally, we show that the reaction product terephthalic acid is pure and obtained in high yields.

The demand for nonwoven materials has increased during the last few years and is expected to increase further due to its use in a broad range of new application areas. Today, the majority of nonwovens are from petroleum‐based resources but there is a desideratum to develop sustainable and competitive materials from renewable feedstock. In this work, renewable nonwovens are produced by solution blowing of dissolved cellulose using 1‐ethyl‐3‐methylimidazolium acetate (EMIMAc) as solvent. Properties of cellulose solutions and process parameters, such as temperature, flow rate, air pressure, and distance to collector, are evaluated in respect to spinnability and material structural properties. Nonwovens with fiber diameters mainly in the micrometer range were successfully produced and it was shown that high temperature or low flow rate resulted in thinner fibers. The produced materials were stiffer (higher effective stress and lower strain) compared to commercial polypropylene nonwoven. © 2019 The Authors. Journal of Applied Polymer Science published by Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48339.