In future biorefineries, the development of inexpensive and renewable reagents for biomass pretreatment is highly desirable.

In recent decades, advancements in lignin application include the synthesis of polymers, dyes, adhesives and fertilizers. There has recently been a shift from perceiving lignin as a waste product to viewing lignin as a potential raw material for valuable products. More recently, considerable attention has been placed in sectors, like the medical, electrochemical, and polymer sectors, where lignin can be significantly valorized. Despite some technical challenges in lignin recovery and depolymerization, lignin is viewed as a promising material due to it being biocompatible, cheap, and abundant in nature. In the medical sector, lignins can be used as wound dressings, pharmaceuticals, and drug delivery materials. They can also be used for electrochemical energy materials and 3D printing lignin–plastic composite materials. This review covers the recent research progress in lignin valorization, specifically focusing on medical, electrochemical, and 3D printing applications. The technoeconomic assessment of lignin application is also discussed.

Despite the enormous potential shown by recent biorefineries, the current bioeconomy still encounters multifaceted challenges. To develop a sustainable biorefinery in the future, multidisciplinary research will be essential to tackle technical difficulties. Herein, we leveraged a known plant genetic engineering approach that results in aldehyde-rich lignin via down-regulation of cinnamyl alcohol dehydrogenase (CAD) and disruption of monolignol biosynthesis. We also report on renewable deep eutectic solvents (DESs) synthesized from phenolic aldehydes that can be obtained from CAD mutant biomass. The transgenic Arabidopsis thaliana CAD mutant was pretreated with the DESs and showed a twofold increase in the yield of fermentable sugars compared with wild type (WT) upon enzymatic saccharification. Integrated use of low-recalcitrance engineered biomass, characterized by its aldehyde-type lignin subunits, in combination with a DES-based pretreatment, was found to be an effective approach for producing a high yield of sugars typically used for cellulosic biofuels and biobased chemicals. This study demonstrates that integration of renewable DES with plant genetic engineering is a promising strategy in developing a closed-loop process. Significance Deep eutectic solvents (DESs) have gained increasing attention due to their application-friendly properties, including universal solvating capabilities and wide tunability. Additionally, ease of synthesis and broad availability from inexpensive chemical components could render DESs more versatile solvents for biomass pretreatment, as compared with traditional ionic liquids. Because the long-term success of the biorefinery depends on the development of sustainable processes to convert lignocellulosics into biofuels, DESs derived from renewable sources such as lignin are highly desirable. We herein present our innovative process that integrates the use of low-recalcitrant engineered biomass with its pretreatment using lignin-derived DESs. The promising results described by near-theoretical sugar yield demonstrate the effectiveness of the integrated process, opening up opportunities toward a sustainable and circular bioeconomy.