Abstract

With the rapid development of the nuclear resource industry, the development of high-efficiency adsorbents is the key to the separation and removal of uranium from aqueous solutions. In this paper, phenyl phosphonic acid was designed as a functional monomer, the aromatic building blocks such as benzene and triptycene as an external crosslinker. Through the “knitting” strategy, a novel phosphonic acid-based functionalized triptycene-based hyper-crosslinked porous polymer (TPP-BPP) and benzene-based hyper-crosslinked porous polymer (B-BPP) were prepared by the above monomer and crosslinker. The resulting polymer B-BPP has a much higher surface area (S_BET = 836.21 m²/g) than that of polymer TPP-BPP (S_BET = 30.60 m²/g) due to the large skeleton triptycene confines the void. Owing to a large number of phosphonic acid functional groups, the polymer TPP-BPP and B-BPP both have a good ability to remove uranium. The optimal adsorption pH is 7 and the adsorption time is 90 min. Under the best experimental conditions, the maximum adsorption capacity of TPP-BPP for uranium is 119.05 mg/g, and the maximum adsorption capacity of B-BPP for uranium is 222.72 mg/g. Furthermore, in the presence of coexisting ions Na⁺, Mg²⁺, Al³⁺, Co²⁺, Ni²⁺, NO³⁻, CO₃²⁻etc., they still have good selectivity to uranium ascribed to the strong complexation between UO₂²⁺ and P=O groups anchored on the polymer, which was evidenced by experimental results. Also, it has good reusability and can still maintain a very high removal percentage after at least being recycled five times. Therefore, the convenient synthesis route for the novel phosphonic acid-based functionalized hyper-crosslinked porous polymer has a promising application prospect for uranium adsorption.

Graphical abstract

中文翻译：

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新型稳健的膦酸官能化芳基超交联多孔聚合物高效去除水溶液中的铀

摘要

随着核资源工业的快速发展，开发高效吸附剂是从水溶液中分离脱除铀的关键。在本文中，苯基膦酸被设计为功能单体，芳香族结构单元如苯和三蝶烯作为外部交联剂。通过“编织”策略，由上述单体和交联剂制备了新型膦酸基功能化三蝶烯基超交联多孔聚合物（TPP-BPP）和苯基超交联多孔聚合物（B-BPP）。所得聚合物 B-BPP 的表面积 ( S _BET  = 836.21 m ² /g) 比聚合物 TPP-BPP ( S _BET  = 30.60 m ^{2 ) 高得多}/g）由于大骨架三蝶烯限制了空隙。由于具有大量的膦酸官能团，聚合物TPP-BPP和B-BPP均具有良好的去铀能力。最佳吸附pH为7，吸附时间为90 min。在最佳实验条件下，TPP-BPP对铀的最大吸附量为119.05 mg/g，B-BPP对铀的最大吸附量为222.72 mg/g。此外，在存在共存离子Na ⁺、Mg ²⁺、Al ³⁺、Co ²⁺、Ni ²⁺、NO ^3-、CO ₃ ^2-等的情况下，由于强络合，它们对铀仍有很好的选择性。 UO _2之间²⁺和 P=O 基团锚定在聚合物上，实验结果证明了这一点。此外，它具有良好的可重复使用性，至少循环使用五次后仍能保持很高的去除率。因此，新型膦酸基官能化超交联多孔聚合物的便捷合成路线在铀吸附方面具有广阔的应用前景。

图形概要