Deep eutectic solvents (DESs) are clean alternatives for chemical reagents and reaction media. Herein, a novel method for zwitterionzation of micro-/nano-cellulose (MC/NC) by a novel ternary DES (TDES) from ZnCl₂, choline chloride (ChCl), and urea was established. In the characterized TDES of ZnCl₂:ChCl:2urea, by phase diagram, viscosity, density, FT-IR, and TGA analyses, ZnCl₃⁻Ch⁺ is hydrogen bond-acceptor (HBA) and two urea molecules are hydrogen bond-donors (HBDs). The theoretical investigations on donor–acceptor mechanism by Functional Density Theory, the reduced density gradient isosurface, and electrostatic potential surface (EPS demonstrate the co-existences of the H-bonding and electrostatic-interactions in formation of ZnCl₂:ChCl:2urea. These interactions between ZnCl₃⁻Ch⁺ complex as HBA and urea HBDs provide a higher equilibrium than the related binary DESs. By this new TDES, alkalized MC or NC was zwitterionized without any additional reagent and the products were characterized by FT-IR, FESEM, EDX, PZC, TGA, and XRD analyses. Dual positively/negatively sites on cellulose and decrease in crystallinity-index (7%) and thermal-stability detected for the given zwitterionized celluloses. In this new protocol, the simply prepared ZnCl₂:ChCl:2urea served as both of reaction medium for dissolution of cellulose and cholinating agent for the zwitterionization of cellulose by nucleophilic attack of the alkalized MC/NC to activated-ChCl by TDES.

低共熔溶剂 (DES) 是化学试剂和反应介质的清洁替代品。_{在此，建立了一种通过ZnCl 2}、氯化胆碱(ChCl)和尿素的新型三元DES (TDES)对微/纳米纤维素(MC/NC)进行两性离子化的新方法。_{在 ZnCl 2} :ChCl:2urea的表征 TDES 中，通过相图、粘度、密度、FT-IR 和 TGA 分析，ZnCl ₃ ⁻ Ch ⁺是氢键受体（HBA），两个尿素分子是氢键供体（HBD）。_{通过功能密度理论、减小的密度梯度等值面和静电势面对供体-受体机制进行理论研究（EPS证明了ZnCl 2} :ChCl:2urea形成过程中氢键和静电相互作用的共存。这些ZnCl ₃ ⁻ Ch ^{+之间的相互作用}HBA 和尿素 HBD 的复合体提供比相关二元 DES 更高的平衡。通过这种新型 TDES，无需任何额外试剂即可对碱化 MC 或 NC 进行两性电离，并通过 FT-IR、FESEM、EDX、PZC、TGA 和 XRD 分析对产品进行表征。对于给定的两性离子化纤维素，检测到纤维素上的双正/负位点以及结晶度指数（7%）和热稳定性的降低。在这个新方案中，简单制备的 ZnCl ₂ :ChCl:2urea 既作为溶解纤维素的反应介质，又作为通过 TDES 亲核攻击碱化 MC/NC 到活化 ChCl 来两性电离纤维素的胆碱剂。