Highly efficient removal of uranium from aqueous solution by a novel robust phosphonic acid functionalized aromatic-based hyper-crosslinked porous polymer

Highly efficient removal of uranium from aqueous solution by a novel robust phosphonic acid functionalized aromatic-based hyper-crosslinked porous polymer
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通过新型稳健的膦酸官能化芳基超交联多孔聚合物从水溶液中高效去除铀

DOI:
10.1007/s10967-022-08395-x
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发表时间:
2022-07
影响因子:
1.6
通讯作者:
Dingzhong Yuan
Dingzhong Yuan
中科院分区:
化学4区
文献类型:
--
作者:
Yan He;Wenli Bao;Bo Li;Xiaolei Fu;Bing Na;Dingzhong Yuan

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随着核资源工业的快速发展,高效吸附剂的开发是从水溶液中分离去除铀的关键。本文设计了以苯基膦酸为功能单体,以苯和三蝶烯等芳香族结构单元为外交联剂。通过“编织”策略,以上述单体和交联剂为原料,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)。由于大骨架三蝶烯限制了空隙,所得聚合物B-BPP具有比聚合物TPP-BPP(SBET= 30.60 m2/g)高得多的表面积(SBET= 836.21 m2/g)。由于TPP-BPP和B-BPP中含有大量的膦酸官能团,因此具有良好的除铀能力。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,在共存离子Na+、Mg 2+、Al 3+、Co2+、Ni 2+、NO3-、CO 32-等的存在下,实验结果表明,由于P=O基团与UO_(2 2+)之间存在较强的络合作用,它们对铀仍具有较好的选择性。此外,它具有良好的可重复使用性,在至少回收五次后仍然可以保持很高的去除率。因此,这种新型膦酸基功能化超交联多孔聚合物的简便合成路线在铀吸附方面具有良好的应用前景。
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 (SBET= 836.21 m2/g) than that of polymer TPP-BPP (SBET= 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
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