Metal–Organic-Framework-Mediated Fast Self-Assembly 3D Interconnected Lignin-Based Cryogels in Deep Eutectic Solvent for Supercapacitor Applications

A cost-effective and sustainable method is successfully developed to produce lignin-based cryogels with a mechanically robust 3D interconnected structure. A choline chloride–lactic acid (ChCl–LA)-based deep eutectic solvent (DES) is used as a cosolvent to promote the synthesis of lignin–resorcinol–formaldehyde (LRF) gels that can self-assemble a robust string-bead-like framework. The molar ratio of LA to ChCl in DES has a significant influence on the gelation time and properties of the ensuing gels. Moreover, it is discovered that doping the metal–organic framework (MOF) during the sol–gel process can greatly accelerate the gelation of lignin. It takes a mere 4 h to complete the LRF gelation process at a DES ratio of 1:5 combined with 5% MOF. This study yields LRF carbon cryogels doped with copper that exhibit 3D interconnected bead-like carbon spheres with a prominent micropore of 1.2 nm. A specific capacitance as high as 185 F g(−1) can be obtained for the LRF carbon electrode at a current density of 0.5 A g(−1), and it has an excellent long-term cycling stability. This study provides a novel method of synthesizing high-lignin-content carbon cryogels with promising potential for application in the field of energy storage devices.