Tailored covalent organic framework with phosphorylation for boosting typical actinide adsorption under acidic conditions
Tailored covalent organic framework with phosphorylation for boosting typical actinide adsorption under acidic conditions
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DOI：
10.1016/j.cej.2023.142408
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发表时间：
2023-03
影响因子：
15.1
通讯作者：
Huidi Zhang;Shuai Wang;Jipan Yu;Zi-jie Li;Jianhui Lan;Lirong Zheng;Siyan Liu;Liyong Yuan
中科院分区：
文献类型：
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作者：
Huidi Zhang;Shuai Wang;Jipan Yu;Zi-jie Li;Jianhui Lan;Lirong Zheng;Siyan Liu;Liyong Yuan
铀和钚是与核燃料循环密切相关的典型锕系元素。在这项工作中，我们合理地设计和制造了一个膦酸基团修饰的共价有机框架，TzDa-Phos，用于高选择性地去除铀[U（VI）]和钚[Pu（IV）]。在pH4.0时，吸附剂对U（VI）的饱和吸附量可达394 mg/g，在1-4 M HNO 3溶液中，吸附剂对U（VI）的饱和吸附量仍保持在40 mg/g。Pu（IV）与TzDa-Phos在3 M HNO 3中的分配系数高达9.7 × 103 mL/g。TzDa-Phos对U（VI）和Pu（IV）的优异吸附性能合理地归因于TzDa中修饰的膦酸基团。具体地说，P双键O与硝酸铀物质的强络合作用（例如，UO 2（NO3）+，UO 2（NO3）20）在高酸度下显示，与FT-IR、XPS和EXAFS分析证明的在pH 4.0下P-O−与铀的配位相反。这项工作提供了一个很有前途的吸附剂回收铀和钚从各种废水通过固相萃取的方法。
Uranium and plutonium are typical actinides tightly associated with nuclear fuel cycle. In this work we rationally design and fabricate a phosphonic group-decorated covalent organic framework, TzDa-Phos, for highly selective removal of uranium [U(VI)] and plutonium [Pu(IV)]. The saturation adsorption capacity for U(VI) can reach 394 mg/g at pH 4.0, and even maintains 40 mg/g in 1–4 M HNO3solutions. The distribution coefficient of Pu(IV) with TzDa-Phos is recorded up to 9.7 × 103mL/g at 3 M HNO3. The excellent adsorption performance of TzDa-Phos for U(VI) and Pu(IV) is reasonably attributed to phosphonic groups decorated in TzDa. Specifically, the strong complexation of Pdouble bondO with uranium nitrate species (e.g., UO2(NO3)+, UO2(NO3)20) is indicated at high acidities, in contrary to the coordination of P-O−with uranium at pH 4.0 as evidenced by FT-IR, XPS and EXAFS analyses. This work provides a promising adsorbent to recover uranium and plutonium from various wastewaters via a solid-phase extraction approach.