Abstract
The post-grafting of porous silica with organic group is a common method for the synthesis of organo-functionalized silica adsorbent. However, this method usually produces adsorbents with limited adsorption performances due to the pore blocking caused by the irregular introduction of organic group. In this work, we report the controllable synthesis of phosphoric acid functionalized porous silica adsorbent based on the co-condensation method for uranium (VI) adsorptive removal with enhanced adsorption performance. Characterizations of the obtained silica verify its porous structure and confirm the homogeneous distribution of phosphoric acid groups inside the silica. This silica is able to efficiently remove 98 % of uranium from a 100 mg/L uranium (VI) solution within 10 min at a dosage of 0.6 g/L and the maximum uranium (VI) adsorption amount reaches 509 mg/g. Both adsorption capacity and adsorption rate of this silica are superior than that of the silica synthesized based on conventional post-grafting method. Moreover, this silica can be reused for five times with uranium (VI) removal efficiency above 95 % and it is well applied in adsorption column for dynamically adsorptive removal of uranium (VI) from real nuclear wastewater. Mechanism-related investigations reveal that uranium (VI) adsorption on this silica proceeds by effective ion exchange of uranium (VI) ion with either phosphoric acid or silanol group and the formation of uranyl phosphonate or uranyl silicate complex. This work provides a feasible strategy to synthesize functionalized porous silica without significant pore blocking, and demonstrates the enhancement effect of regulating surface adsorption groups on the adsorption performances of porous silica. Besides, this work offers a promising adsorbent for efficient treatment of uranium-containing nuclear wastewater and reveals the mechanism of uranium adsorption on those silica adsorbent containing phosphoric acid, thiol or thioether group.
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