• Optimal solvothermal separation (GVL/H2O, 60% GVL, 205°C, 1.7 h) yields wheat straw cellulose with 89.4% purity and 86.7% recovery.
• High fractional separation efficiency (purity × recovery) and low crystallinity of cellulose synergistically enhance HMF yield.
• Drying of separated cellulose (heat or freeze) re-crystallizes it, reducing HMF yield; wet cellulose gives 58.6% HMF molar yield, 1.5× higher than microcrystalline cellulose.
• The study underscores avoiding drying steps in cellulose biorefinery to maintain reactivity for HMF production.
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